Solar-driven photocatalytic water splitting paves a way to produce green hydrogen for building a sustainable clean energy system, particularly within the framework of the carbon-neutral initiative. However, to date, the solar-to-hydrogen (STH) conversion efficiency of particulate photocatalysts falls far short of the demand of over 10% for industrial applications. Single-domain ferroelectric semiconductor materials with amazing unidirectional spontaneous polarization penetrating the bulk are promising candidates as photocatalysts for water splitting. Their existing inherent internal field set up by polarization can cause both two oppositely charged surfaces (namely, polar surfaces) and spatial separation of photogenerated charge carriers between them upon light excitation. These unique properties provide sufficient new room for flexibly engineering of bulk and surface/interface structures to enhance photocatalytic water splitting.

Bacterial infections pose an ongoing threat to global human health, an issue of growing urgency due to the emergence of resistance against many currently available antibiotics. Recently, the World Health Organization (WHO) launched a global appeal for the development of novel antibiotics to combat this issue. Ideal antibiotics should possess specific antibacterial effects, without causing resistance. However, the discovery of different antibiotics is lagging the development of drug-resistant bacteria. Many newly developed antibiotics not only are rapidly resisted by bacteria but also are ineffective against persistent bacteria embedded in biofilms and host cells. To tackle these challenges, innovative concepts and approaches are required for the discovery of novel antibacterial candidates.

Optical imaging with high spatiotemporal resolution has been developed as a vital technology to reveal biological mysteries. Researchers have made countless profound innovations to promote the investigations on cell biology, especially after the implementation of far-field optical super-resolution imaging technology. Intrinsically, in-depth understanding of physiological activities inevitably requires optical imaging in living organisms at tissue, cell, or even single molecule levels. However, such a requirement usually encounters a great bottleneck because traditional optical imaging has little ability to penetrate biological tissues. Recently, the newly emerged optical imaging technology based on the second near-infrared window (NIR-II, 1000∼1700 nm) has changed this predicament. With suppressed light-scattering and diminished tissue autofluorescence, NIR-II optical imaging can easily achieve micrometer scale resolution at sub-centimeter tissue depth. Therefore, researchers regard it as a new avenue for in vivo optical imaging research.

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Figure 1. (a) Guidelines for the construction of HTP physical fields; region I represents energy density, region II represents the power of energy input, and region III represents an insulated space without external energy input. (b) General strategy for providing faster PHT physical fields. (c) Typical time-dependent temperature profile during HTP. (d) Characteristics of HTP in the synthesis of kinetically controlled products being trapped at various local minima relative to the thermodynamic product located at the global minimum in terms of the total free energy. Reproduced with permission from ref (16). Copyright 2021 American Chemical Society. (e) Space-time scales for a heterogeneous catalytic process. The light red represents the process of chemical dynamics on the catalyst, the light green region represents the molecular reaction process, and the light blue region represents the transport processes of the reactants. Reproduced with permission from ref (17). Copyright 2015 John Wiley & Sons, Inc. (f) Synthesis of intermediate and metastable structures by using pulsed heating methods. (g) Time-temperature transformation diagram showing the kinetic formation of metallic glass, high entropy alloy, and phase-separated structures, respectively, as a function of cooling rate. Reproduced with permission from ref (10). Copyright 2018 The Authors. Figure 2. (a) Typical space-time scales for different heating methods and fundamental processes occurs during materials synthesis. (b) Size-controlled synthesis of Pt-based materials by tuning the duration of HTP, a faster heating/cooling rate and a shorter HTP generate smaller particles. (b1) Pt foil. Reproduced with permission from ref (19). Copyright 2018 The Authors. (b2) Pt NPs. Reproduced with permission from ref (20). Copyright 2020 American Chemical Society. (b3) Pt clusters. Reproduced with permission from ref (21). Copyright 2020 John Wiley & Sons, Inc. (b4) Pt SAs. Reproduced with permission from ref (22). Copyright 2019 The Author(s). (c) Composition-controlled synthesis of high-entropy materials; the rapid cooling process enabled a homogeneous mixture of various elements into one particle while preventing phase separation. (c1) Schematic of the high-entropy mixing in a face-centered cubic lattice. Multiple elements will occupy the same lattice site randomly to form a high-entropy structure such as a high-entropy alloy. Reproduced with permission from ref (14). Copyright 2022 The Authors. (c2) Schematic of a HEA nanoparticle. Reproduced with permission from ref (14). Copyright 2022 The Authors. (c3) Schematic of an HEO nanoparticle. Reproduced with permission from ref (25). Copyright 2021 The Author(s). (c4) Schematic of an HEC nanoparticle. (d) Phase-controlled synthesis of molybdenum carbide materials by tuning the peak temperature of HTP. Reproduced with permission from ref (27). Copyright 2022, The Author(s). (d1) β-Mo2C, (d2) α-MoC1–x, (d3) η-MoC1–x. (e) Morphology-controlled synthesis of Si nanostructures; graphene interlayer confined (e1) Si NPs. Reproduced with permission from ref (28). Copyright 2016, The Author(s). (e2) Si NWs. Reproduced with permission from ref (29). Copyright 2021 John Wiley & Sons, Inc. Figure 3. (a) Prevalent and laboratory-achievable energy ranges of thermal energy, electrical energy, and light energy; electrical and light energy can drive chemical reactions with ΔG > 0 while thermal energy cannot. (b) Typical time scales involved in various pulsed heating methods. (c) Construction of laser-triggered HTP by various types of photothermal mechanisms in carbonaceous materials, semiconductor materials, and plasmonic metal materials such as Au, Ag, Cu, etc. Reprinted with permission from ref (32). Copyright 2019 Royal Society of Chemistry. (d) Excitation and relaxation of surface plasmons, as well as the corresponding three main effects, including the enhanced electromagnetic near field, excited carriers (e– refers to electron and h+ is hole) and local heating. Reprinted with permission from ref (34). Copyright 2023 Springer Nature Limited. The utilization of operando characterization and data-driven computational analysis for establishing the synthesis–structure–performance relationship. The significance of advanced characterization under realistic operando HTP conditions and high-throughput computational analysis is increasingly recognized as it provides a scientific basis for the development of innovative solid catalyst materials, chemical processes, or systems. This approach is expected to address the limitations of empirical schemes and effectively satisfies multiple catalytic performance objectives. The comprehensive comprehension of the multifield coupling effect toward the synthesis of solid catalysts by pulsed heating. The generate and application of HTP in the preparation of solid catalysts are typically accompanied by the presence of various physical fields, including electrical, magnetic, and optical fields. However, the extent to which these fields can impact the synthesis of solid catalysts remains largely unknown. Controllable synthesis of designed solid catalysts through the implementation of programmable pulsed heating methods. The development of programmable pulsed heating techniques with high levels of temporal and spatial accuracy is imperative in expediting the shift from traditional trial-and-error methodologies toward novel paradigms for the development of exceptional and sustainable solid catalysts. Scalable and cost-effective synthesis of function-specific solid catalyst materials by automated and continuous pulsed heating approach. In forthcoming times, it is imperative to prioritize the large-scale manufacturing of sophisticated solid catalysts by pulsed heating strategy, which satisfies the criteria of industrial catalytic applications, namely high-performance and low cost. Ye-Chuang Han received his Ph.D. degree from Xiamen University in 2022 under the supervision of Prof. Zhong-Qun Tian. He is now a postdoctoral fellow at Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province under the supervision of Prof. Zhong-Qun Tian. His work focuses on synthetic chemistry under extreme environments. Pei-Yu Cao received her B.S. degree from Hubei University in 2023. She is currently a M.S. student at Xiamen University under the supervision of Prof. Zhong-Qun Tian. Her work focuses on ultrafast materials synthesis and processing. Zhong-Qun Tian received his B.S. degree at Xiamen University in 1982 and his Ph.D. degree under the supervision of Prof. Martin Fleischmann at the University of Southampton in 1987. He has been a full Professor of Chemistry at Xiamen University since 1991. He is a Member of the Chinese Academy of Sciences and the Elected President of the International Society of Electrochemistry. Currently, his main research interests include surface enhanced Raman spectroscopy, spectroelectrochemistry, nanochemistry, plasmonics, catalyzed molecular assembly, and synthetic chemistry under extreme environments. We sincerely thank Prof. Yanan Chen from Tianjin University and Prof. Yonggang Yao from Huazhong University of Science and Technology for their insightful discussions. This work was supported by the China Postdoctoral Science Foundation (2022M722646), the National Natural Science Foundation of China (21991130), and the National Key Research and Development Program of China (2021YFA1201502). This article references 34 other publications. This article has not yet been cited by other publications. Figure 1. (a) Guidelines for the construction of HTP physical fields; region I represents energy density, region II represents the power of energy input, and region III represents an insulated space without external energy input. (b) General strategy for providing faster PHT physical fields. (c) Typical time-dependent temperature profile during HTP. (d) Characteristics of HTP in the synthesis of kinetically controlled products being trapped at various local minima relative to the thermodynamic product located at the global minimum in terms of the total free energy. Reproduced with permission from ref (16). Copyright 2021 American Chemical Society. (e) Space-time scales for a heterogeneous catalytic process. The light red represents the process of chemical dynamics on the catalyst, the light green region represents the molecular reaction process, and the light blue region represents the transport processes of the reactants. Reproduced with permission from ref (17). Copyright 2015 John Wiley & Sons, Inc. (f) Synthesis of intermediate and metastable structures by using pulsed heating methods. (g) Time-temperature transformation diagram showing the kinetic formation of metallic glass, high entropy alloy, and phase-separated structures, respectively, as a function of cooling rate. Reproduced with permission from ref (10). Copyright 2018 The Authors. Figure 2. (a) Typical space-time scales for different heating methods and fundamental processes occurs during materials synthesis. (b) Size-controlled synthesis of Pt-based materials by tuning the duration of HTP, a faster heating/cooling rate and a shorter HTP generate smaller particles. (b1) Pt foil. Reproduced with permission from ref (19). Copyright 2018 The Authors. (b2) Pt NPs. Reproduced with permission from ref (20). Copyright 2020 American Chemical Society. (b3) Pt clusters. Reproduced with permission from ref (21). Copyright 2020 John Wiley & Sons, Inc. (b4) Pt SAs. Reproduced with permission from ref (22). Copyright 2019 The Author(s). (c) Composition-controlled synthesis of high-entropy materials; the rapid cooling process enabled a homogeneous mixture of various elements into one particle while preventing phase separation. (c1) Schematic of the high-entropy mixing in a face-centered cubic lattice. Multiple elements will occupy the same lattice site randomly to form a high-entropy structure such as a high-entropy alloy. Reproduced with permission from ref (14). Copyright 2022 The Authors. (c2) Schematic of a HEA nanoparticle. Reproduced with permission from ref (14). Copyright 2022 The Authors. (c3) Schematic of an HEO nanoparticle. Reproduced with permission from ref (25). Copyright 2021 The Author(s). (c4) Schematic of an HEC nanoparticle. (d) Phase-controlled synthesis of molybdenum carbide materials by tuning the peak temperature of HTP. Reproduced with permission from ref (27). Copyright 2022, The Author(s). (d1) β-Mo2C, (d2) α-MoC1–x, (d3) η-MoC1–x. (e) Morphology-controlled synthesis of Si nanostructures; graphene interlayer confined (e1) Si NPs. Reproduced with permission from ref (28). Copyright 2016, The Author(s). (e2) Si NWs. Reproduced with permission from ref (29). Copyright 2021 John Wiley & Sons, Inc. Figure 3. (a) Prevalent and laboratory-achievable energy ranges of thermal energy, electrical energy, and light energy; electrical and light energy can drive chemical reactions with ΔG > 0 while thermal energy cannot. (b) Typical time scales involved in various pulsed heating methods. (c) Construction of laser-triggered HTP by various types of photothermal mechanisms in carbonaceous materials, semiconductor materials, and plasmonic metal materials such as Au, Ag, Cu, etc. Reprinted with permission from ref (32). Copyright 2019 Royal Society of Chemistry. (d) Excitation and relaxation of surface plasmons, as well as the corresponding three main effects, including the enhanced electromagnetic near field, excited carriers (e– refers to electron and h+ is hole) and local heating. Reprinted with permission from ref (34). Copyright 2023 Springer Nature Limited. This article references 34 other publications.

All-solid-state lithium batteries have received considerable attention in recent years with the ever-growing demand for efficient and safe energy storage technologies. However, key issues remain unsolved and hinder full-scale commercialization of all-solid-state lithium batteries. Previously, most discussion only focused on how to achieve high energy density from the theoretical perspective. Herein, we analyze the real cases of different kinds of all-solid-state lithium batteries with high energy density to understand the current status, including all-solid-state lithium-ion batteries, all-solid-state lithium metal batteries, and all-solid-state lithium–sulfur batteries. First, we propose a general calculation method to visually compare the above battery systems partly due to no normative parameters for solid-state batteries. After then, we discuss and interpret the key parameters and current situation of all-solid-state lithium batteries. Through the summary and analysis of the frontier, one can find that, although some breakthrough has been made in energy density and areal capacity for solid-state batteries, there are still many aspects to be improved such as power density and rate performance. Therefore, in response to the challenges, we propose possible directions for future development, including the ways to prepare different kinds of solid electrolyte films to reduce the proportion of inactive substances in the cell. The advantages and disadvantages are discussed about three typical solid-state electrolyte films (inorganic solid electrolyte, solid polymer electrolyte, and composite solid electrolyte). In addition, potential candidate anodes with high capacity and cathodes with high voltage and/or high capacity are also discussed in details. The combination of lithium metal anodes with ultrahigh capacity and cathodes with both high capacity and high voltage is the current mainstream direction. However, the interface problems have become the most pressing factor on the application. Therefore, we introduce the origin of interfaces and interphases and discuss how to build a stable electrode/solid electrolyte interface. One thing is clear that artificial solid electrolyte interphases and composite solid electrolytes are effective to obtain stable anode/solid electrolyte interfaces, which can prevent lithium from constantly reacting with solid electrolytes, ensure the uniform lithium deposition and prevent the formation of lithium dendrites. For the cathode/solid electrolyte interface, reasonable composite cathodes, multilayer design, and composite solid electrolytes can optimize the electrode and interface for stable cycles at high voltages and high current densities. Furthermore, the contribution of high-throughput computations and machine learning is introduced in accelerating materials screening and development. Among them, progress has been made in solid electrolytes and artificial solid electrolyte interphases through materials genome engineering and machine learning. Finally, we provide some outlook for the future development. We hope that this Account could help understand the current status and inspire more future breakthrough for all-solid-state lithium batteries.

The carbon balance has been disrupted by the widespread use of fossil fuels and subsequent excessive emissions of carbon dioxide (CO2), which has become an increasingly critical environmental challenge for human society. The production and use of renewable energy sources and/or chemicals have been proposed as important strategies to reduce emissions, of which the electrochemical CO2 (or CO) reduction reaction (CO2RR/CORR) in the aqueous systems represents a promising approach.

Cucurbit[7]uril (CB[7]), an important member of the macrocyclic cucurbit[n]uril host family, has attracted much attention due to its ability to form ultrastable inclusion complexes with aromatic or “ring”-structured compounds. In particular, for the CB[7]@ferrocene (Fc) host–guest complex, its exceptionally high binding affinity, ideal redox activity, and extreme stability against biological media have promoted its potential to substitute traditional natural binding pairs (antigen/antibody and biotin/avidin complexes as examples) in many biochemical applications, such as purification, labeling, and biomolecular assembly. In recent years, the immobilization of CB[7]@Fc host–guest complex on electrode surface via various strategies has expanded its use for fabricating electroactive biofunctional devices, such as electrochemical biosensors and switches, where the redox response of Fc/Fc+ can be used as both characterization and sensing signal. These applications require in-depth understanding of the interfacial CB[7]@Fc host–guest binding behavior, which is different from that in a homogeneous solution phase; such studies, in turn, will facilitate the design and development of more efficient interfacial host–guest binding systems.

Hydrogen is deemed as an ideal energy carrier because of its high energy density and clean nature. Water electrolysis is fairly competitive for hydrogen production due to the conversion of renewable electricity to high-purity H2 with no carbon emission, in comparison with traditional industrial technology. However, the large-scale application is hampered by high cost partially from the use of noble metal-based catalysts to promote the kinetics of hydrogen and oxygen evolution reactions. Developing cost-efficient transition metal-based electrocatalysts, therefore, is a hopeful prospect, because they can provide d-orbital lone-pair electrons or empty d-orbitals for adsorbing different intermediates (such as H*, OH*, O*, and OOH*). As compared to transition metals and their oxides, transition metal interstitial compounds (TMICs) formed by inserting C, N, and P atoms into the interstitial sites of parent metals hold distinct advantages in their Pt-like electronic structure, high conductivity, and superior chemical stability over a wide pH range, beneficial to overcoming the high energy consumption faced by alkaline water electrolysis and the intractable stability issue of acid water electrolysis. Nevertheless, the major drawbacks are large size, high density, and sluggish ionic kinetics, resulting in ordinary electrochemical activity and low mass efficiency. Electrocatalytic performance is dominated by the intrinsic activity, the number of accessible active sites, and the capacity of charge and mass transfer. Engineering the micronano structure (small-size particles, porous structure, and ultrathin nanosheet) can expose more catalytical active sites and facilitate mass transport and gas diffusion. Meanwhile, modulating the electronic structure can optimize the adsorption energy of the intermediates to boost the intrinsic activity. Apparently, synergistic modulation of the micronano structure and electronic structure of TMICs is expected to achieve the multiobjective optimization for targeting the highly effective catalysts.

Supported metal catalyst, has been one of the most important systems in the field of heterogeneous catalysis. The great complexity of both the compositions and structures of such supported metal catalysts provides a great degree of freedom for tuning their catalytic properties, which has essentially triggered the explosive growth in research on design and control active metals’ surface structures for decades. An ideal metal catalyst theoretically features maximum active sites and optimal intrinsic reactivity to facilitate a desired chemical reaction. Inspired by the catalytic concepts brought by natural enzymes and homogeneous catalysis, the fabrication of heterogeneous catalysts with atomically dispersed metal atoms has attracted much attention and been extensively explored in recent years.

Solar energy is one of the most promising energy sources to replace traditional fossil fuels due to its renewable and green features, which can be converted to electrical and chemical energy through photon-enabled applications. To improve the utilization efficiency of solar energy, solar energy “converters”, such as photovoltaic and photocatalytic systems, have been extensively studied. It is noteworthy that the common issues of narrow optical absorption and rapid charge carrier recombination limit solar energy utilization. The development of advanced functional nanomaterials plays a decisive role in addressing these issues. For instance, plasmonic nanomaterials with a localized surface plasmon resonance (LSPR) effect can effectively extend and enhance light absorption; heterojunction- and homojunction-based semiconductors can facilitate the spatial separation of electron–hole pairs. Therefore, rational design of functional nanomaterials through integrating plasmonic nanomaterials and creating heterojunctions and homojunctions can amplify their structural advantages, leading to the achievement of the state-of-the-art photon-conversion performance. Besides, the in-depth understanding of the relationship between materials and performance via advanced characterization techniques, such as high spatial-resolution imaging and in situ spectroscopy, provides a fundamental and solid basis for optimizing advanced functional materials in photon-enabled applications. Along with theoretical calculation and algorithm-driven data analysis during advanced characterizations, more quantified information can be obtained for deeper insights into physics. In this Account, we first summarize recent works in our research group on the rational design of advanced functional materials, including plasmonic metallic materials, plasmonic semiconductors, two-dimensional-material-based heterojunctions, and metal–organic-framework-based homojunctions, and their working mechanisms for the enhancement of photovoltaic and photocatalytic performance. We then show how we employed developed X-ray-based, electron-based, and spectroscopic techniques for characterizing elemental composition, materials structure, and physicochemical properties, which provides effective ways to resolve complex structures and processes and understand their underlying physics. Furthermore, we discuss the photogenerated charge carrier dynamics in solar cells and photocatalysis using in situ and time-resolved techniques, by underlining the use of these advanced techniques for specific materials. Then, we briefly introduce the algorithm-driven data analysis compiled in analytical techniques in our works to quantify materials information. Finally, we briefly present perspectives for addressing the challenges and fundamental issues as well as guidance for the future development of photon-enabled applications, e.g., the development of high-performance functional materials and advanced characterization techniques. This Account shows some ideas and directions for the rational design and optimization of advanced functional materials for various photon-enabled applications and for the proper utilization of advanced characterization techniques, which may provide guidance and prospects for future research.

Programmable engineered tissues and the materials that support them are instrumental to the development of next-generation therapeutics and gaining new understanding of human biology. Toward these ends, recent years have brought a growing emphasis on the creation of “4D” hydrogel culture platforms─those that can be customized in 3D space and on demand over time. Many of the most powerful 4D-tunable biomaterials are photochemically regulated, affording users unmatched spatiotemporal modulation through high-yielding, synthetically tractable, and cytocompatible reactions. Precise physicochemical manipulation of gel networks has given us the ability to drive critical changes in cell fate across a diverse range of distance and time scales, including proliferation, migration, and differentiation through user-directed intracellular and intercellular signaling. This Account provides a survey of the numerous creative approaches taken by our lab and others to recapitulate the dynamically heterogeneous biochemistry underpinning in vivo extracellular matrix (ECM)–cell interactions via light-based network (de)decoration with biomolecules (e.g., peptides, proteins) and in situ protein activation/generation. We believe the insights gained from these studies can motivate disruptive improvements to emerging technologies, including low-variability organoid generation and culture, high-throughput drug screening, and personalized medicine. As photolithography and chemical modification strategies continue to mature, access to and control over new and increasingly complex biological pathways are being unlocked.

The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/accountsmr.2c00221. Discussion on the activation of CuO cathode by Bi-based additive inclusions (Supplementary Note 1), challenges of MZIB cathodes (Supplementary Note 2) and meeting the challenge of developing highly reversible Zn anodes (Supplementary Note 3), AZB cathode mechanism schematic, SEM and TEM images, electronic mapping images and ex situ data, galvanostatic (curve/cycling) data for AZB/MZIBs, Zn anode printing schematic, performance data for AZBs/MZIBs and optic microscopy images (PDF) Electronic Supporting Information files are available without a subscription to ACS Web Editions. The American Chemical Society holds a copyright ownership interest in any copyrightable Supporting Information. Files available from the ACS website may be downloaded for personal use only. Users are not otherwise permitted to reproduce, republish, redistribute, or sell any Supporting Information from the ACS website, either in whole or in part, in either machine-readable form or any other form without permission from the American Chemical Society. For permission to reproduce, republish and redistribute this material, requesters must process their own requests via the RightsLink permission system. Information about how to use the RightsLink permission system can be found at http://pubs.acs.org/page/copyright/permissions.html.

Two-dimensional (2D) semiconducting materials are poised to revolutionize ultrathin, high-performance optoelectronic devices. In particular, transition-metal dichalcogenides (TMDs) are well-suited for applications requiring robust and stable materials such as electrocatalytic, photocatalytic, and photo-electrochemical devices. One of the most compelling assets of these materials is the ability to produce and process 2D TMDs in the nanosheet form using solution-based (SB) exfoliation methods. Compared to other methods, SB techniques are typically inexpensive, efficient, and more suitable for scale-up and industrial implementation. In acknowledgment of the importance of this area, much work has been done to develop various SB methods starting from the exfoliation of bulk crystalline TMD materials to the chemical modification of final devices consisting of thin films of semiconducting 2D TMD nanosheets. However, not all SB methods are equally compatible or interchangeable, and they result in very diverse material and device properties. Therefore, the aim of this Account is to provide an overview of the developed SB techniques that can serve as a guide for assembling high-performance thin films of 2D TMDs. We start by introducing the most popular methods for producing 2D TMDs using liquid-phase exfoliation (LPE), discussing their working mechanisms as well as their advantages and disadvantages. Notably we highlight a recently developed LPE technique using electro-intercalation that draws on the advantages of previously presented methods. Next, we discuss processing the as-produced 2D TMD nanosheets via SB separating techniques designed for size and morphology selection while also presenting the ongoing challenges in this area. We then examine SB methods for processing the selected 2D nanomaterial dispersions into semiconducting thin films. Various methods are compared and contrasted, and special attention is paid to a recently developed method that carefully deposits 2D TMD nanoflakes with preferential alignment and has been shown scalable to the meter-squared size range. Finally, we explore strategies for increasing the optoelectronic performance of the TMD films via device engineering and defect management. We scrutinize these post-treatments based on the final device application, which are explicitly discussed. In all of the discussed processes we present the most promising SB techniques giving critical analysis and insight from experience. While we provide our own “best practices”, we stress the use of adaptability and critical thinking when designing specifically tailored procedures. By providing examples of different uses and measured improvements in one comprehensive guide, we hope to simplify process-development and aid researchers in making their own unique photoactive 2D “puzzles”.

After developments in just more than a decade, the power conversion efficiency (PCE) of single junction perovskite solar cells (PSCs) has achieved a record of 26.0%. Such rapid progress of PSCs technology is mainly attributed to the excellent optoelectronic properties and facile solution-processed fabrication. Starting from the birth of PSCs up to present, various methods have been attempted to improve the performance and/or stability of PSCs. The first perovskite photovoltaic devices achieved a very low efficiency, attributed to the poor quality of the perovskite film upon a mesoporous substrate. There then are large amounts of work aiming at high-quality light-absorber films with pin-free, dense, homogeneous morphology with high crystallinity. Hereafter, the developments of carrier transport materials/layers (CTLs) based on different device structures had become an important issue. The stable CTLs with excellent electrical properties and matched energy levels are desired for efficient and stable PSCs. Besides perovskite film growth control and employment of advanced CTLs, the main studies are mitigation of all kinds of defects in PSCs, including charge traps in the perovskite bulk, interface defects between the perovskite and adjacent CTLs, and grain boundaries located at dangling bonds as well as halide loss defects. All of these defects in PSCs can not only cause nonradiation recombination but also provide an extra pathway for ionic migration, which leads to irreversible degradation of the perovskite film. And the very current studies on defects are trying to push PSCs to industrial application, since the long-term stability and high-efficiency count as the same importance for PSCs. There is an apparent fact that the literature about PSC fabrication is based on different experiment conditions, which gives it poor reproducibility. Herein, the conception and motivation of the studies are more valuable. It is necessary to share the research in detail by individual laboratories for a better communication in this rapidly developed field. It could be concluded that there are mainly three steps for PSCs to achieve such high-efficiency and appreciable stability: 1) modulation of the perovskite film quality; 2) development of desired CTLs for PSCs; 3) mitigation of defects in the perovskite bulk and/or interfaces. The three steps are also the basic development track of PSCs. In this Account, we will briefly review the milestones in the early period of PSCs. Then, we will mainly focus on our group and coauthors’ representative progress of high-efficiency PSCs, following the above development order of PSCs technology. The mechanisms and motivations of improved efficiency and stability in different stages are discussed. Finally, a comprehensive summary as well as the deep perspectives of PSCs are proposed. And the future directions of PSCs for practical application are also discussed.

Two-dimensional (2D) semiconducting transition metal dichalcogenides (TMDs) have demonstrated exceptional potential as materials for future complementary metal-oxide-semiconductor (CMOS) technology. This is primarily because of their atomic thickness and excellent electrical and mechanical properties. With advancements in fabrication technology, electronic devices based on 2D TMD materials have rapidly progressed from isolated units for scientific experimentation to integrated circuits with practical applications. Among the different production methods, the solution-processing of 2D TMD nanomaterial dispersions offers the distinct advantages of low-temperature processing and cost-effective manufacturing for large-scale flexible and wearable electronics. A wide range of 2D nanoflake inks with versatile electronic properties can be assembled into atomic-thick thin films with dangling-bond-free van der Waals interfaces between adjacent nanoflakes. Furthermore, direct printing techniques can easily integrate multifunctional devices, such as n-type and p-type transistors, into CMOS devices and more complex integrated circuits. Despite these benefits and previous accomplishments, the field of solution-processed CMOS electronics using 2D TMD semiconducting materials is in its early stages of development and requires further research. One of the current challenges is the production of scalable and high-purity 2D semiconductor mono- and few layers with large lateral sizes and narrow thickness distribution. The field-effect mobility of solution-processed 2D TMD transistors remains lower than that of the transistors manufactured using mechanical exfoliation and chemical vapor deposition methods. In particular, limited research has been conducted on solution-processed p-type 2D TMD transistors. As a result, solution-processed CMOS devices using n-type and p-type 2D TMD transistors are scarce. In this Account, we provide an overview of the recent progress in the field of solution-processed CMOS electronics employing 2D TMD materials. First, we introduce the basic liquid exfoliation methods, such as sonication-assisted exfoliation and molecular intercalation methods, that are commonly utilized to prepare 2D TMD dispersions. In addition, we discuss the production of monolayer 2D materials, which serve as the building blocks for fabricating atomic-thick thin films. Subsequently, we review the typical techniques for depositing 2D inks, including spin coating, drop casting, and inkjet printing. Furthermore, we outline the thin-film patterning process for each technique, which is crucial for integrating multifunctional materials in CMOS devices. Subsequently, we focus on the recent advancements in solution-processed 2D TMD transistors. Furthermore, we explore the various factors that can improve the performance of the devices with regard to charge transport and charge traps. Afterward, we highlight notable applications of solution-processed CMOS technology, such as logic circuits and ring oscillators. Finally, we provide an overview of the challenges and opportunities in the development of solution-processed 2D materials and the integration of multifunctional devices for the advancement of CMOS electronics. This Account aims to provide a comprehensive guide for readers, offering both a broad overview and an in-depth insight into solution-processed 2D material-based electronics, covering a wide range of topics from the preparation of 2D TMD ink to device fabrication and CMOS applications. Therefore, this Account is expected to drive further progress and advancements in this field and promote the realization of practical applications.

Solid catalysts play a key role in the chemical industry, energy, and the environment. Fundamental understanding of heterogeneous catalysis exerted by solid surfaces is useful for structural designs of efficient catalysts but is challenging due to the complexity. Emerging uniform catalytic nanocrystals (NCs) with controlled and well-defined surface structures have brought new opportunities for fundamental understanding and directed explorations of efficient catalysts. In a previous Account ( Acc. Chem. Res. 2016, 49, 520−527), I postulated and exemplified a concept of oxide nanocrystal model catalysts for the fundamental investigations of oxide catalysis without the “materials gap” and “pressure gap” which are often encountered using the traditional single crystal model catalysts. In this Account, I summarize our effort in fabricating efficient uniform nanocrystal catalysts based on the fundamental understanding of structure–activity relations and reaction mechanisms acquired by oxide nanocrystal model catalyst studies. Directed by the fundamental understanding that the Cu2O{110} facet is active in catalyzing propylene epoxidation with O2 and the fine Cu2O nanocube exposes high densities of Cu2O{110} edge sites, we successfully explore fine Cu2O nanocubes as a highly selective catalyst for propylene epoxidation with O2. Directed by the fundamental understanding that the Cu{100} facet is the active Cu facet in catalyzing the water–gas shift (WGS) reaction, we successfully fabricate a highly active ZnO/fine Cu nanocube WGS catalyst with enhanced ZnO-CuCu{100} active site density. Directed by the fundamental understanding of TiO2 facet effects on the surface band bending and adsorbate–surface interfacial energy level alignment, and consequent photocatalytic performance, we successfully fabricate highly active TiO2{001} NC-based photocatalysts for photocatalytic CH4 conversions. These results adequately exemplify the concept of fundamental understanding-directed explorations of efficient catalysts following a strategy of “identification of active site structure + maximization of active site density”, which, together with the advancement of controlled-synthesis methods, is expected to greatly accelerate the explorations of novel and efficient catalysts in future.

Tremendous progress in nanomaterial and nanotechnology has been made in recent years, which greatly contributes to the development of inorganic nanoparticles (NPs) as luminescent probes in diverse biomedical applications. In particular, these luminescent nanoprobes are widely employed for sensitive assays of biomarkers like disease markers. Generally, the luminescent bioassay technologies mainly rely on conventional molecular probes such as lanthanide (Ln3+) chelates or organic dyes, which suffer from inferior photochemical stability, low photobleaching, potential long-term toxicity, or high background noise. In contrast, Ln3+-doped NPs possess distinct physicochemical properties including better photostability, lower toxicity, and superior optical properties like long photoluminescent (PL) lifetime, narrow emission band, and tunable spectral range from the ultraviolet to the second near-infrared (NIR-II), which make them extremely ideal as luminescent nanoprobes. As such, enormous research enthusiasm has been invested in this fascinating field of Ln3+-doped luminescent nanoprobes in recent years. Accordingly, background-free luminescent bioassays with high signal-to-noise have been achieved by employing Ln3+-doped NPs on the basis of their downshifting luminescence (DSL) with a long PL lifetime, NIR-II luminescence with long-wavelength emissions, or upconverting luminescence (UCL) upon NIR excitation. However, there are still key challenges for Ln3+-doped nanoprobes owing to their low brightness and quantum yield, which restrict their biomedical applications. During the past decade, we have explored efficient approaches for the synthesis and design of highly efficient Ln3+-doped nanoprobes toward ultrasensitive luminescent bioassay of disease markers.

Figure 1. (A) Different emulsions (w/o, o/w, o/o, and multi-) stabilized by small molecule or polymeric surfactants. (B) Cartoon with routes of polymerization to produce of foams (open/closed cell), capsules, and armored particles. Figure 2. Modification of graphene oxide (GO) by reaction with primary alkyl amines to give nanosheets of different wettability for stabilization of nonaqueous emulsions. Functionalization of GO with hexyl amine gives nanosheets dispersible in DMF and capable of stabilizing octane-in-DMF o/o emulsions (left). Functionalization of GO with octadecyl amine gives nanosheets dispersible in octane and capable of stabilizing DMF-in-octane o/o emulsions (right). Optical microscope images reproduced with permission from ref (40). Copyright 2017 American Chemical Society. Figure 3. Examples of the performance of composite structures produced from Pickering emulsions: (A) Capsules of ionic liquid (IL) and their performance in uptake of CO2: (i) comparison of capacity of still IL, agitated IL, and encapsulated IL, (ii) time for equilibration of CO2 uptake for agitated IL and encapsulated IL, and (iii) CO2 uptake and release profiles for capsules with core of task specific IL. (3Ai-3Aii) reproduced with permission from ref (22). Copyright 2019 American Chemical Society. (3Aiii) reproduced with permission from ref (46). Copyright 2019 American Chemical Society. (B) Capsules with core of salt hydrate phase change material (PCM): (i) optical microscopy image of capsules when heated about the melting point of the PCM, (ii) DSC curve of bulk PCM, and (iii) DSC trace of encapsulated PCM. Reproduced from ref (48) with permission. Copyright 2022 Elsevier. (C) Capsules with a shell that contains hindered urea bonds: (i) optical microscopy image of as prepared capsules, (ii) SEM image of capsules after shell fusion, and (iii) optical microscopy image of the emulsion formed after destruction of shells. Reproduced with permission from ref (50). Copyright 2022 American Chemical Society. Emily Pentzer is an associate professor in the Department of Chemistry and Department of Materials Science & Engineering at Texas A&M University, with a courtesy appointment in the Department of Chemical Engineering. She received her B.S. in Chemistry from Butler University (2005) and PhD in Chemistry from Northwestern University (2010), then performed postdoctoral research at UMass Amherst in Polymer Science and Engineering. She started her independent career at Case Western Reserve University and moved her group to Texas A&M in 2019. The Pentzer Lab’s research focuses on developing new polymeric materials and assemblies as a route to understand structure–property–application relationships and access functions not possible with current state-of-the-art systems. Dr. Pentzer was named an ACS WCC Rising Star and Texas A&M Presidential Impact Fellow. She currently serves as an associate editor for the RSC journal Polymer Chemistry and is editor in chief of RSC Applied Polymers. Eliandreina Cruz Barrios received her B.S. in Chemistry (2008) from University of Carabobo, M.S. in Chemistry (2014), with focus on colloidal and interface science, from Venezuelan Institute of Scientific Research, and PhD in Chemistry (2022) from Texas Christian University; she is currently a Postdoctoral Researcher at Texas A&M University under the supervision of Dr. Emily Pentzer. Her research focuses on microencapsulation strategies using multiple emulsions. Nicholas Starvaggi received his B.S. in chemistry and biochemistry from Mount St. Mary’s University in 2021. He is currently pursuing his PhD in Chemistry in the Pentzer lab at Texas A&M University, where he is an NSF graduate research fellow. His research interests focus on functionalized soft materials and microencapsulation strategies. E.P. acknowledges NSF DMR #2103182. E. C. B. acknowledges DEEE0009155 for funding. N.S. is supported by NSF GRFP #2139772. This article references 52 other publications. This article has not yet been cited by other publications. Figure 1. (A) Different emulsions (w/o, o/w, o/o, and multi-) stabilized by small molecule or polymeric surfactants. (B) Cartoon with routes of polymerization to produce of foams (open/closed cell), capsules, and armored particles. Figure 2. Modification of graphene oxide (GO) by reaction with primary alkyl amines to give nanosheets of different wettability for stabilization of nonaqueous emulsions. Functionalization of GO with hexyl amine gives nanosheets dispersible in DMF and capable of stabilizing octane-in-DMF o/o emulsions (left). Functionalization of GO with octadecyl amine gives nanosheets dispersible in octane and capable of stabilizing DMF-in-octane o/o emulsions (right). Optical microscope images reproduced with permission from ref (40). Copyright 2017 American Chemical Society. Figure 3. Examples of the performance of composite structures produced from Pickering emulsions: (A) Capsules of ionic liquid (IL) and their performance in uptake of CO2: (i) comparison of capacity of still IL, agitated IL, and encapsulated IL, (ii) time for equilibration of CO2 uptake for agitated IL and encapsulated IL, and (iii) CO2 uptake and release profiles for capsules with core of task specific IL. (3Ai-3Aii) reproduced with permission from ref (22). Copyright 2019 American Chemical Society. (3Aiii) reproduced with permission from ref (46). Copyright 2019 American Chemical Society. (B) Capsules with core of salt hydrate phase change material (PCM): (i) optical microscopy image of capsules when heated about the melting point of the PCM, (ii) DSC curve of bulk PCM, and (iii) DSC trace of encapsulated PCM. Reproduced from ref (48) with permission. Copyright 2022 Elsevier. (C) Capsules with a shell that contains hindered urea bonds: (i) optical microscopy image of as prepared capsules, (ii) SEM image of capsules after shell fusion, and (iii) optical microscopy image of the emulsion formed after destruction of shells. Reproduced with permission from ref (50). Copyright 2022 American Chemical Society. This article references 52 other publications.

Organic electronics has experienced substantial advances in the past decade, driven by the development of high-performance organic semiconductors (OSCs) in combination with device engineering. While the pursuit of new aromatic building blocks has been a central topic in OSC innovation, the installation of novel side chains is also of significance for accessing high-performance solution-processable OSCs due to their great impact on (macro)molecular conformation/configuration, energy levels, intra/intermolecular interaction, and packing motifs, as well as film morphology of the materials.