Cyclic voltammetry (CV) is a powerful technique for characterizing the electrochemical properties of electrochemical devices. During charging–discharging cycles, the thermal effect can have a profound effect on its performance. However, existing theoretical models cannot clarify such an intrinsic mechanism and often give poor predictions. Herein, we propose an interfacial model for the electro-thermal coupling based on fundamentals in nonequilibrium statistical mechanics. By incorporation of molecular interactions, our model shows a quantitative agreement with experimental measurements. The integral capacitance shows a first enhanced and then decayed trend against the applied heat bath temperature. Such a relation is attributed to the competition between electrical attraction and Born repulsion via dielectric inhomogeneity, which was not well understood in previous models. In addition, as evidenced in recent experimental CV tests, our model predicts the nonmonotonic dependence of the capacitance on the bulk electrolyte density. This work demonstrates a potential pathway toward next-generation thermal regulation of electrochemical devices.

Metallic Zn anodes exhibit uncontrollable dendrites, impractically low Zn utilization, hydrogen evolution, and unexpected byproducts, limiting the practical process of aqueous zinc-ion batteries (AZIBs); thus, exploring alternative insertion anodes has become a reasonable strategy, exemplified by the successful application of graphite anodes in lithium-ion batteries. However, the current intercalative anodes are still plagued by high Zn2+ insertion potential and inadequate cycle life, and the alternative choice is quite limited. Here, we report a polyanionic insertion anode (Ti2O(PO4)2·2H2O) that shows an extremely low insertion potential of 0.07 V with a reversible capacity of 124.6 mAh g–1. This anode possesses a robust and spacious framework, demonstrating high reversibility with low strain during cycling. Coupled with a KZnHCF cathode, a 1.6 V “rocking-chair” full battery is achieved with an ultralong life of 5000 cycles, surpassing the reported congeneric batteries. This work shares a new vision for the development of practical AZIBs.

All-inorganic wide-bandgap (WBG) perovskite solar cells are best suited as the top cells for tandem devices. However, they suffer from photoinduced halide segregation (PIHS) and a quick anion exchange reaction (AER). Herein, polyvinylpyrrolidone (PVP) polymer-assisted in situ crystalization of CsPbBr3 and CsPbBr1.5I1.5 compounds is shown to suppress these effects by passivation of both positively charged (halide vacancy) and negatively charged (cation vacancy) defects. Modifying the perovskite precursor solution with this polymer improved the chemical stability and photostability in both nanocrystal solution and solution-processed films. Ultrafast transient absorption measurements elucidate the excited state dynamics of PVP-modified perovskite and probe an improved lifetime of charge carriers. As a proof of concept, PVP-modified CsPbI1.5Br1.5 retained nearly 98% Voc and 90% PCE under 1 sun AM 1.5G illumination for 12 h, while the control devices lost 25% of their Voc within 6 h. Using simple polymer additives to protect WBG perovskites is a huge step toward new device architectures involving all-perovskite heterojunctions.

The aprotic Li–CO2 battery provides a tantalizing solution for simultaneous CO2 capture and electrical energy storage. Nevertheless, current Li–CO2 batteries based on ordinary reaction pathways, e.g., reducing CO2 to CO, oxalate, carbon, etc., often suffer from poor energy efficiency and severe parasitic reactions. Thus, exploring new Li–CO2 electrochemistry is of fundamental interest and practical importance. Herein, we report a new concept of a Li–CO2 battery that can realize both reversible capture/release of CO2 and highly efficient energy storage based on the redox cycle of 4,4′-bipyridine (BPD). Direct spectroscopic evidence coupled with theoretical calculations reveals that BPD first coordinates with CO2 to form a [BPD···2CO2] complex that can further be reduced via a two-electron pathway into Li2[BPD-2CO2] upon discharge; upon recharge the reaction is reversed, regenerating BPD and CO2. The BPD-assisted Li–CO2 battery minimizes the overpotential required to drive the discharge/charge reaction, eliminates the undesired parasitic reactions associated with pristine Li–CO2 batteries, and delivers a high discharge capacity (>1000 mAh/gc). This work represents a significant step forward toward truly reversible Li–CO2 batteries by the rational design of redox molecules that can participate in and regulate the conventional Li–CO2 electrochemistry.

Organic redox-active molecules are promising materials for charge storage in redox-flow batteries (RFBs); however, the development of all-organic RFBs is hindered by material crossover, limited energy density, and poor stability of active materials. Here, ester-substituted bispyridinylidenes are reported as the first examples of intrinsic bipolar molecules that exhibit basically concerted double two-electron redox activity at a potential difference of 1.01 V. All three oxidation states of the pentylester derivative exhibited excellent temporal stability and good solubility in the electrolyte. Testing this active material in symmetric cells, which alleviates crossover issues, revealed good cyclability (fade of 0.025% and 0.35% per cycle for static and flow cells, respectively), capacities of up to 89% of the theoretical value, and Coulombic efficiencies above 99%. Considering previous evidence for active material solubility limits of ∼2 M, and the benefits of a symmetric design, such double concerted multielectron bipolar active materials will be key to developing energy dense organic RFBs.

We develop an adaptive machine-learning framework that addresses cross-operation-condition battery lifetime prediction, particularly under extreme conditions. This framework uses correlation alignment to correct feature divergence under fast-charging and extremely fast-charging conditions. We report a linear correlation between feature adaptability and prediction accuracy. Higher adaptability generally leads to better prediction accuracy, aiding efficient feature engineering. Our analysis shows that the first 120 cycles provide sufficient information for lifetime prediction, and extending data to the first 320 cycles only marginally improves prediction accuracy. An early prediction using only one feature at the 20th cycle produces a 93.3% accuracy, saving up to 99.4% computation time and repetitive tests. Our quantitative adaptability evaluation enhances prediction accuracy while reducing information redundancy via proper feature and cycle selections. The proposed framework is validated under another unseen complex operation condition with a 90.3% accuracy without prior knowledge.

Quasi-two-dimensional (2D) Pb–Sn mixed perovskites show great potential in applications of single and tandem photovoltaic devices, but they suffer from low efficiencies due to the existence of horizontal 2D phases. Here, we obtain a record high efficiency of 18.06% based on 2D ⟨n⟩ = 5 Pb–Sn mixed perovskites (iso-BA2MA4(PbxSn1–x)5I16, x = 0.7), by optimizing the crystal orientation through a regulation of the Pb/Sn ratio. We find that Sn-rich precursors give rise to a mixture of horizontal and vertical 2D phases. Interestingly, increasing the Pb content can not only entirely suppress the unwanted horizontal 2D phase in the film but also enhance the growth of vertical 2D phases, thus significantly improving the device performance and stability. It is suggested that an increase of the Pb content in the Pb–Sn mixed systems facilitates the incorporation of iso-butylammonium (iso-BA+) ligands in vertically oriented perovskites because of the reduced lattice strain and increased interaction between the organic ligands and inorganic framework. Our work sheds light on the optimal conditions for fabricating stable and efficient 2D Pb–Sn mixed perovskite solar cells.

Sorption-based atmospheric water harvesting (AWH) is regarded as a promising way to produce fresh water in water-stressed areas. However, low water production per unit device mass (WPD) and high energy consumption restrict its applications in portable fresh water replenishment. Here we report a portable high-yield AWH device based on a thermoelectric cell (TEC)-driven integrated heating/cooling thermal design, enabled by a thermally tailored hydrogel sorbent. Heat and cold energies for desorption and condensation are simultaneously generated by the TEC. Graphene oxide-doped sodium alginate hydrogel with high thermal conductivity is tailored as the sorbent, which tightly adheres to the TEC’s hot region and efficiently takes heat away, for fast desorption as well as temperature control of the TEC. Based on the thermal design of the device and materials, a total WPD of 0.18 L kgdevice–1 h–1 is achieved under 80% RH, almost an order of magnitude higher than that of the traditional design with the same energy input.

Gas-fed flow cells can facilitate high-rate electrochemical CO2 reduction (CO2R). However, under alkaline and neutral conditions, CO2 is lost through reaction with hydroxide ions to form (bi)carbonate. In acidic solutions, although (bi)carbonate is still formed due to increased pH at the electrode, the low bulk pH of the electrolyte solution can regenerate CO2 which is then available for re-reaction or release─this therefore avoids permanent CO2 loss. Here, we show how CO2 is converted and released in a bipolar-membrane-based gas-fed flow cell for CO2R to multicarbon products (C2+ faradaic efficiency >60%) employing an acidic catholyte. Under the highest conversion conditions, we showed that almost exclusively CO2R products were obtained at one outlet, while, at the second outlet, a nearly product-free stream of CO2 was obtained due to the continuous internal regeneration from (bi)carbonate. The system presented here avoids permanent reactant loss through the straightforward recovery and recycling of CO2 to improve the overall CO2 utilization.

We present a recyclable perovskite–graphene heterostructure that demonstrates ultrahigh X-ray detection sensitivities over 108 μC/Gyair·cm2 for medical imaging applications. The high mobility of the graphene pixel is preserved to over 1200 cm2/V·s after perovskite deposition and enables large conversion efficiency for ultrahigh sensitivity. Increasing the operational bias of the graphene channel increased the X-ray detection signal-to-noise ratio from 30 to over 200. The perovskite can be washed off by an organic solvent at room temperature without damaging the graphene. Redepositing the perovskite layer retains the detectors’ high gain, making our heterostructure X-ray detector a recyclable device. The perovskite–graphene device exhibits robust operation given 10,000 gate sweeps and multicycle X-ray irradiations. Here we have demonstrated a high-performance, low-cost, plug-and-play solution with a recyclable design that could significantly reduce the manufacturing and maintenance costs associated with X-ray cameras in medical imaging.

Pulsed electrocatalysis has emerged as a promising technology to effectively improve reaction kinetics and tailor product selectivity. While most research focuses on the evolution of electrocatalyst active sites, the dynamic response of the interfacial microenvironment during pulsed electrocatalysis still remains unknown. Here, we reveal the in situ dynamic regulation of the interfacial microenvironment induced by pulsed electrocatalysis in the oxygen reduction reaction process, from the interface reactant delivery to intermediate formation dynamics. At the diffusion layer, the coupling of pulsed electrocatalysis and hierarchical pore structure was proven to break the limitation of proton transfer, resulting in favorable H2O2 production kinetics. At the electrode/electrolyte interface, the pulsed electric field would stimulate the cation effect to activate C–*OOH and reduced the reaction energy barrier, giving rise to more favorable *OOH formation thermodynamics. This work provides new insights into exploring in situ regulation of the interfacial microenvironment, which is expected to be extended to different electrochemical processes.

Anion-exchange membrane water electrolysis (AEM-WE) promises low cost, green hydrogen production for the future. In order to meet this potential, significant improvements to the performance and stability of catalyst layers (CLs) must be made, including the development of tailor-made ion conducting polymer materials. This Focus Review outlines the role of anion-exchange ionomers (AEIs) in CLs for enabling catalyst activation, enhancing stability toward delamination, and improving ion conduction. Detrimental effects such as inhibition of the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) and oxidative instability of the ionomer are also discussed with key findings from recent AEM-WE literature. Opportunities for future ionomer development are discussed to guide such efforts.

Figure 1. The importance of nanomaterials and sustainability to science and technology is schematically illustrated via the interconnections of three topical areas: Nanostructured Materials for Sustainable Energy Solutions, Nano-bio Hybrid Materials for Energy and CO2 Reduction, and Sustainable Manufacturing at the Nanoscale. Figure 2. Diagram showing different pump–probe techniques and the information obtained from each technique. Figure 3. (Top) Assembly of a nano-bio hybrid. (Bottom left) Proposed mechanism of photosynthetic CO2 reduction to value-added chemicals by a nano-bio hybrid. (Bottom right) Photocatalytic CH4 and CO formation under various conditions. Adapted from ref (14). Copyright 2019 American Chemical Society. Figure 4. Schematics of a graphene/nanodiamond-based superlubric solid lubricant coating developed at Argonne National Laboratory showing application from (a) solution to (b) bearing. The schematic in (c) shows a diamond-like carbon (DLC) ball sliding on nanodiamond/graphene patches. Adapted from ref (16). Copyright 2015 American Association for the Advancement of Science. Figure 5. 2030 cumulative iridium demand. Conservative at 80–100 GW at 40% PEM; aggressive at 80% PEM. Work at the Center for Nanoscale Materials, a U.S. Department of Energy Office of Science User Facility, was supported by the U.S. DOE, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. Material from P.K.J. is based upon work supported by the National Science Foundation under Grant No. CHE-2304910. The work of H.X. was supported by the U.S. National Science Foundation Grant Nos. DMR-1408949, 1454984, and 1838604. R.B. thanks the Graduate School NANO- PHOT (École Universitaire de Recherche, contract ANR-18-EURE-0013) for support. This article references 20 other publications. This article has not yet been cited by other publications. Figure 1. The importance of nanomaterials and sustainability to science and technology is schematically illustrated via the interconnections of three topical areas: Nanostructured Materials for Sustainable Energy Solutions, Nano-bio Hybrid Materials for Energy and CO2 Reduction, and Sustainable Manufacturing at the Nanoscale. Figure 2. Diagram showing different pump–probe techniques and the information obtained from each technique. Figure 3. (Top) Assembly of a nano-bio hybrid. (Bottom left) Proposed mechanism of photosynthetic CO2 reduction to value-added chemicals by a nano-bio hybrid. (Bottom right) Photocatalytic CH4 and CO formation under various conditions. Adapted from ref (14). Copyright 2019 American Chemical Society. Figure 4. Schematics of a graphene/nanodiamond-based superlubric solid lubricant coating developed at Argonne National Laboratory showing application from (a) solution to (b) bearing. The schematic in (c) shows a diamond-like carbon (DLC) ball sliding on nanodiamond/graphene patches. Adapted from ref (16). Copyright 2015 American Association for the Advancement of Science. Figure 5. 2030 cumulative iridium demand. Conservative at 80–100 GW at 40% PEM; aggressive at 80% PEM. This article references 20 other publications.

With the advent of nonfullerene acceptors (NFAs), organic photovoltaic (OPV) devices are now achieving high enough power conversion efficiencies (PCEs) for commercialization. However, these high performances rely on active layers processed from petroleum-based and toxic solvents, which are undesirable for mass manufacturing. Here, we demonstrate the use of biorenewable 2-methyltetrahydrofuran (2MeTHF) and cyclopentyl methyl ether (CPME) solvents to process donor: NFA-based OPVs with no additional additives in the active layer. Furthermore, to reduce the overall carbon footprint of the manufacturing cycle of the OPVs, we use polymeric donors that require a few synthetic steps for their synthesis, namely, PTQ10 and FO6-T, which are blended with the Y-series NFA Y12. High performance was achieved using 2MeTHF as the processing solvent, reaching PCEs of 14.5% and 11.4% for PTQ10:Y12 and FO6-T:Y12 blends, respectively. This work demonstrates the potential of using biorenewable solvents without additives for the processing of OPV active layers, opening the door to large-scale and green manufacturing of organic solar cells.

The solvent-free manufacturing process for battery electrodes has gathered increased scientific interest due to its cost reduction, eco-friendliness, and ability to enhance electrode density. Carbon nanotubes (CNTs) are anticipated to improve battery performance, owing to their exceptional electrical conductivity and unique one-dimensional morphology. In this study, we demonstrate that the integration of ozone treatment for CNTs can further enhance the electrochemical performance of high-loading (30 mg/cm2 or higher) dry-processed cathodes employing high-nickel active materials (NCM811). By comparing these cathodes with dry-processed cathodes using carbon black, a conventional conductive agent, we elucidate that the enhanced performance of single-walled (SW) CNT-based cathodes originates from the formation of a cathode-electrolyte interphase with favorable protective abilities and the capacity to suppress microcrack formation within NCM811 particles. The current study presents a promising strategy of incorporating SWCNTs with the tuned surface functionalities for the development of cost-effective, environmentally friendly dry battery manufacturing.

A multiscale water visualization technique for polymer electrolyte fuel cells was established by using operando multiprobe radiography with pulsed spallation neutron and synchrotron X-ray sources. The three-dimensional water distribution revealed that water back-diffusion from the cathode to the anode significantly contributes to the “drainability” of practical polymer electrolyte fuel cells toward fuel cell electric vehicles.

Efficient desolvation and fast lithium ion (Li+) transport are key factors for fast-charging Li metal batteries (LMBs). Here, we report a self-assembled interphase (SAI) with ordered Li+ transport pathways to enable high Li+ conductivity and fast Li+ desolvation for fast-charging LMBs. A self-assembled structure originating from the intermolecular π–π stacking endows SAI with ordered Li+ transport pathways. The regular molecular stacking and a gradient distribution of functional groups of SAI contribute to a spatially confined gradient desolvation of Li+. Thereby, a stable Li metal anode (LMA) with durable solid-electrolyte interphase, accelerated Li+ transfer, and homogeneous Li plating/stripping is achieved at high rates. A full-cell battery of SAI protected LMA|LiNi0.8Co0.1Mn0.1O2 delivers a high capacity of 147 mAh g–1 with an improved capacity retention for 500 cycles at 3 C (1 C = 210 mA g–1), and the full cell can deliver over 71% of its capacity in 12 min.

We modify the PEDOT:PSS hole transport layer (HTL), commonly adopted for high-performance tin perovskite solar cells (TPSCs), via post-treatment of its surface using aromatic diammonium acetate salts dissolved in a highly volatile but interactive solvent. The solvent partly etches excessive insulating PSS while enabling tight anchoring of the salts to the PEDOT:PSS HTL. The salts improve not only the PEDOT:PSS/perovskite interface but also the top surface of tin perovskite thin films, leading to reduced interface defects, larger built-in potentials, and suppressed perovskite pinhole defects. In addition, the salts transform the PEDOT structure from benzoid to quinoid and depopulate excessive hole charge carriers to promote hole extraction. Consequently, TPSCs attain a high efficiency of 12.1% under standard 1 sun light illumination and impressive stability without encapsulation for ∼2800 h under an N2 atmosphere. We developed a straightforward but impactful method to modify PEDOT:PSS for broader applications.

Single-atom catalysts (SACs) are being widely developed for the CO2 reduction reaction (CO2RR) because of their remarkable activity and selectivity. However, insufficient CO2RR performance and the poor long-term stability of the SACs remain obstacles to process scale-up. Herein, we explore Ni SACs (Ni-N/NCNT) under practical conditions using a zero-gap CO2 electrolyzer for CO production. We demonstrate that the CO2RR performance of the Ni-N/NCNT results from the suitable Ni–N–C, which enhanced electron transfer and increased CO2 adsorption. Furthermore, we propose a strategy for improving the CO2RR performance and long-term stability by focusing on the membrane electrode assembly (MEA) structure. A maximum Faradaic efficiency of 96.73% (at 2.1 V) and partial current density of 219.49 mA cm–2 (at 2.4 V) for CO production were obtained on the MEA with the Ni-N/NCNT catalyst and the Sustainion (Sust.) membrane. In addition, MEA with Sust. exhibited long-term stability at −100 mA cm–2 for over 60 h.

Given the great potential for achieving record breaking organic solar cells (OSCs), newly explored solid additives that could optimize nanoscale morphology of active layers have rapidly gained widespread attention. Herein, a new volatile solid additive 2,5-dichlorothieno[3,2-b]thiophene (TT-Cl) is delicately explored, fully satisfying the design criteria of a planar conjugated skeleton with suitable molecular size, symmetrical geometry, and proper halogenation. When applied in the state-of-the-art OSCs with diverse active layers, the quite high crystallinity of TT-Cl and strong interactions with light-harvesting components lead to optimized molecular crystalline ordering, fibrillar networks, and vertical phase distributions, thus offering a significant performance enhancement. Consequently, PM6:Y6-based binary and ternary OSCs achieved PCEs of 18.20% and 18.95%, respectively. Moreover, PM6:CH23-based binary OSCs presented an outstanding PCE of 18.72%. Our work not only provides a broad-spectrum solid additive to optimize film morphologies powerfully but also manifests great potential for achieving a record-breaking PCE of OSCs.