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| Open AccessTuning polymer-backbone coplanarity and conformational order to achieve high-performance printed all-polymer solar cells
All-polymer solar cells comprising both polymeric donors and acceptors offer better morphological and mechanical stability, and a broader processing window for printing. Here, the authors report a polymer acceptor based on bithiazole linker with more coplanar and ordered molecular conformation.
- Yilei Wu
- , Yue Yuan
- & Zhenan Bao
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Article
| Open AccessDeciphering the contributing motifs of reconstructed cobalt (II) sulfides catalysts in Li-CO2 batteries
Improving catalyst efficiency is vital for Li-CO2 batteries, but understanding catalyst structures during battery operation is hard. Here, the authors uncover catalyst reconstruction and its link to activity, highlighting a self-constructed oxysulfide structure with high activity and stability in Li-CO2 batteries.
- Yingqi Liu
- , Zhiyuan Zhang
- & Hui-Ming Cheng
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Article
| Open AccessA Ce-CuZn catalyst with abundant Cu/Zn-OV-Ce active sites for CO2 hydrogenation to methanol
Carbon dioxide hydrogenation is an important industrial reaction. Here, the authors design a CeCuZn catalyst through a metal organic framework template for CO2 hydrogenation to methanol with excellent methanol yield and stability.
- Runping Ye
- , Lixuan Ma
- & Jian Liu
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Article
| Open AccessProton-selective coating enables fast-kinetics high-mass-loading cathodes for sustainable zinc batteries
Sluggish Zn2+-dominated Faradic reactions lead to suboptimal charge-storage capacity and durability of aqueous zinc battery cathodes. Here, the authors present a proton-selective interfacial coating strategy that enables high-performance cathodes with fast-kinetics proton-dominated Faradic reactions.
- Quanquan Guo
- , Wei Li
- & Xinliang Feng
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Article
| Open AccessInter-site structural heterogeneity induction of single atom Fe catalysts for robust oxygen reduction
Here, authors report an inter-site structural heterogeneity induced effect of hierarchical single atom Fe catalysts for robust oxygen reduction. Dynamic evolutions and insights into structure-activity relationship are presented.
- Peng Zhang
- , Hsiao-Chien Chen
- & Yuan Pan
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Article
| Open AccessSupramolecular catalyst with [FeCl4] unit boosting photoelectrochemical seawater splitting via water nucleophilic attack pathway
The strongly coupled interface between molecular catalysts and light absorbers is the key to solving efficient photoelectrochemical water oxidation. An in situ polymerized supramolecular-like catalyst was used to couple with BiVO4 for efficient and stable photoelectrochemical seawater splitting
- Jiaming Miao
- , Cheng Lin
- & Kan Zhang
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Article
| Open AccessMolecular anchoring of free solvents for high-voltage and high-safety lithium metal batteries
Advanced electrolyte is essential for high-energy-density lithium metal batteries. Here, the authors design a molecular anchoring dilute electrolyte via intermolecular hydrogen bonding with free solvents to improve the battery electrochemical and thermal stabilities.
- Zhuangzhuang Cui
- , Zhuangzhuang Jia
- & Xiaodi Ren
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Article
| Open AccessThe dynamic adsorption affinity of ligands is a surrogate for the passivation of surface defects
Semiconductor defects persist as a source of energy loss in solar cells. Here, the authors use ab initio simulations to reveal overlooked defect dynamics, guiding passivator design for enhanced photovoltaic performance.
- Jian Xu
- , Aidan Maxwell
- & Edward H. Sargent
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Article
| Open AccessPolymer-acid-metal quasi-ohmic contact for stable perovskite solar cells beyond a 20,000-hour extrapolated lifetime
The development of robust quasi-ohmic contact with minimal resistance, exceptional stability and cost-effectiveness is crucial for practical application of perovskite solar cells. Here, authors report a polymer-acid-metal structure as the contact and realize long photo-thermal-operational stability.
- Junsheng Luo
- , Bowen Liu
- & Yicheng Zhao
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Article
| Open AccessDynamic chloride ion adsorption on single iridium atom boosts seawater oxidation catalysis
The seawater oxidation reaction faces challenges from competitive chloride oxidation reaction. Herein, the authors have utilized chlorine adsorption to modulate the single-atom Ir coordination state and promote seawater oxidation and catalyst stability.
- Xinxuan Duan
- , Qihao Sha
- & Xiaoming Sun
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Article
| Open AccessEfficient all-small-molecule organic solar cells processed with non-halogen solvent
The development of non-halogen solvent processed all-small-molecule organic solar cells was challenging. Here, the authors employ a small molecule donor with strong aggregation property to improve molecular pre-aggregation in tetrahydrofuran, realizing ternary device with efficiency of 16.1%.
- Wei Gao
- , Ruijie Ma
- & Gang Li
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Article
| Open AccessAn acetate electrolyte for enhanced pseudocapacitve capacity in aqueous ammonium ion batteries
Ammonium ion batteries are of growing interest for energy storage research. Here, the authors observe two-step pseudocapacitive storage behavior in an ammonium acetate electrolyte, resulting in a superior ammonium ion storage capacity.
- Zhuoheng Bao
- , Chengjie Lu
- & ZhengMing Sun
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Article
| Open AccessModelling atomic and nanoscale structure in the silicon–oxygen system through active machine learning
Understanding the silicon-oxygen system is crucial for various applications. Here, the authors present an interatomic potential covering a wide range of the Si-O configurational space and showcase applications to silica and Si-SiO2 interfaces.
- Linus C. Erhard
- , Jochen Rohrer
- & Volker L. Deringer
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Article
| Open AccessCation desolvation-induced capacitance enhancement in reduced graphene oxide (rGO)
Understanding local electrochemical processes can help improve electrochemical energy storage. Here, the authors report a charge storage mechanism in aqueous electrolyte for reduced graphene oxide using an electrochemical quartz crystal microbalance.
- Kangkang Ge
- , Hui Shao
- & Patrice Simon
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Article
| Open AccessCharging modulation of the pyridine nitrogen of covalent organic frameworks for promoting oxygen reduction reaction
The catalytic efficacy of covalent organic frameworks (COFs) is constrained by their restricted electro-transfer capability and weak binding affinities for reaction intermediates. Here the authors report COFs with various pyridinic-based units for tuning their catalytic activity towards oxygen reduction reaction.
- Xiubei Yang
- , Qizheng An
- & Gaofeng Zeng
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Article
| Open AccessRational molecular and device design enables organic solar cells approaching 20% efficiency
A systematic design of light-absorbing molecules is challenging for them to satisfy multiple key requirements for efficient solar cell application. Here, the authors optimize halogen substitution position in terminal groups of acceptors for realizing ternary cells with efficiency approaching 20%.
- Jiehao Fu
- , Qianguang Yang
- & Gang Li
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Article
| Open AccessSingle-atom tailored atomically-precise nanoclusters for enhanced electrochemical reduction of CO2-to-CO activity
Tailoring catalytic performance of atomically-precise metal nanoclusters catalysts is of great interest but remains challenging. Here, the authors report a co-eletropolymerization strategy to modify well-defined Au8 nanoclusters by single-atom sites to enhance its electrocatalytic activity for the reduction of CO2 towards CO.
- Yi-Man Wang
- , Fang-Qin Yan
- & Shuang-Quan Zang
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Article
| Open AccessContinuous strain tuning of oxygen evolution catalysts with anisotropic thermal expansion
Tuning compressive strain is an effective way to accelerate the oxygen evolution reaction kinetics. Here the authors show that anisotropic thermal expansion induces compressive strains on IrO6 octahedron in Sr2IrO4, shifting its d-band center downward and accelerating water oxidation kinetics beyond traditional thermal diffusion effects.
- Yu Du
- , Fakang Xie
- & Zhigang Zou
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Article
| Open AccessDistance effect of single atoms on stability of cobalt oxide catalysts for acidic oxygen evolution
Dissolution of Co atoms in acidic media impedes the application of cobalt oxides in proton exchange membrane water electrolyzers. Here, the authors reveal a stabilizing effect induced by Ir single atoms on cobalt oxides that suppress Co dissolution.
- Zhirong Zhang
- , Chuanyi Jia
- & Jie Zeng
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Article
| Open AccessEngineering surface dipoles on mixed conducting oxides with ultra-thin oxide decoration layers
Improving materials for energy devices relates to an optimisation of their surfaces. Here authors show that surface modification with ultrathin oxide layers allows for a tailoring of the surface dipole and the work function of mixed ionic and electronic conducting oxides.
- Matthäus Siebenhofer
- , Andreas Nenning
- & Markus Kubicek
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| Open AccessIn situ copper faceting enables efficient CO2/CO electrolysis
Copper electrocatalysts enable carbon dioxide/carbon monoxide reduction but suffer from low production rates. Here, the authors promote in situ growth of Cu(100) during electrolysis, enabling efficient and stable electrosynthesis of multicarbon products at industrially-relevant current densities
- Kaili Yao
- , Jun Li
- & Hongyan Liang
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Article
| Open AccessToward stabilization of formamidinium lead iodide perovskites by defect control and composition engineering
The black phase formamidinium lead iodide perovskite (α-FAPbI3) undergoes an undesired transformation to a non-perovskite δ-phase, rendering it inactive. Here authors show the significant role of inherent iodine defects in accelerating phase transition kinetics and exacerbating α-FAPbI3 instability.
- Yuhang Liang
- , Feng Li
- & Rongkun Zheng
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Article
| Open AccessCoverage enhancement accelerates acidic CO2 electrolysis at ampere-level current with high energy and carbon efficiencies
The increased surface coverage of CO2 electroreduction (CO2R) intermediates promotes CO2R at high operating current densities under strongly acidic conditions. Here the authors report a 77.4% single-pass carbon efficiency for conversion of acidic CO2R to pure formic acid.
- Xiaohan Yu
- , Yuting Xu
- & Miao Zhong
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Article
| Open AccessEfficient direct repairing of lithium- and manganese-rich cathodes by concentrated solar radiation
Rapid capacity decay and voltage drop hinder lithium- and manganese-rich cathode material (LMRO) development. Here, the authors apply concentrated solar radiation arrays on cycled LMRO electrodes, inducing inverse spinel phase to boost redox activity and reversibility, yielding enhanced electrochemical performance.
- Hailong Wang
- , Xin Geng
- & Xin He
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Article
| Open AccessLiquid metal-embraced photoactive films for artificial photosynthesis
The practical applications of photoelectrochemical water splitting pivot on significant advances that enable scalable production of robust photoactive films. Here, the authors propose a proof-of-concept for fabricating bioinspired robust photoactive films by a particle implanting technique, which embeds semiconductor photoabsorbers in the liquid metal.
- Chao Zhen
- , Xiangtao Chen
- & Gang Liu
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Article
| Open AccessUnveiling the nature of Pt-induced anti-deactivation of Ru for alkaline hydrogen oxidation reaction
Despite the high intrinsic activity of Ru for hydrogen oxidation reaction, the surface oxidation-induced deactivation limits the application. Here, the authors report the introduction of Pt atoms could prevent the surface oxidation-related interfacial water network damage, preventing the deactivation of Ru.
- Yanyan Fang
- , Cong Wei
- & Gongming Wang
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Article
| Open AccessGeneral synthesis and atomic arrangement identification of ordered Bi–Pd intermetallics with tunable electrocatalytic CO2 reduction selectivity
Precise synthesis of Intermetallic compounds and understanding of the structure-performance correlation are highly desirable in catalysis. Here, the authors develop a general method to synthesize up to six BiPd intermetallic compounds and study the mechanism toward the electrocatalytic carbon dioxide reduction reaction.
- Wenjin Guo
- , Guangfang Li
- & Rong Chen
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Article
| Open AccessSuperexchange-stabilized long-distance Cu sites in rock-salt-ordered double perovskite oxides for CO2 electromethanation
Cu-oxide-based catalysts are promising for CO2 electromethanation but suffer from inevitable reduction and structural collapse. Here the authors report a Cu-based rock-salt-ordered double perovskite oxide with superexchange-stabilized long-distance Cu sites for efficient and stable CO2 methanation.
- Jiawei Zhu
- , Yu Zhang
- & Heqing Jiang
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Article
| Open AccessStable water splitting using photoelectrodes with a cryogelated overlayer
Photoelectrodes made of earth-abundant materials can contribute to low-cost and carbon-free hydrogen production, but suffer from a short lifetime. Here the authors report cryogel overlayer to increase the operation time of the device by regulating evolving hydrogen bubble dynamics.
- Byungjun Kang
- , Jeiwan Tan
- & Hyungsuk Lee
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Article
| Open AccessKirkendall effect-induced uniform stress distribution stabilizes nickel-rich layered oxide cathodes
Nickel-rich layered oxide cathodes offer high energy density yet suffer from mechanical degradation during (de)lithiation. Here, the authors present a strategy that leverages the Kirkendall effect to equalize stress within the cathode particles, thereby stabilizing their structure and enhancing the cycling stability.
- Ziyao Gao
- , Chenglong Zhao
- & Baohua Li
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Article
| Open AccessPromoting high-voltage stability through local lattice distortion of halide solid electrolytes
Solid electrolytes play a crucial role as ion conductors and separator between electrodes in all-solid-state batteries. Here, the authors report a high-entropy halide solid electrolyte, which reveals the structure evolution with the increasing configurational entropy and improves the high-voltage stability.
- Zhenyou Song
- , Tengrui Wang
- & Wei Luo
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Article
| Open AccessElucidation of the role of metals in the adsorption and photodegradation of herbicides by metal-organic frameworks
In this study, the authors explored the correlation between the structure and optoelectronic properties of metal organic frameworks for the removal of a harmful herbicide from water.
- Nan Chieh Chiu
- , Jacob M. Lessard
- & Kyriakos C. Stylianou
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Article
| Open AccessOxygen-tolerant CO2 electroreduction over covalent organic frameworks via photoswitching control oxygen passivation strategy
Direct use of flue gas for the electrocatalytic CO2 reduction reaction is desirable but severely limited by the thermodynamically favorable oxygen reduction reaction. Here the authors report an oxygen passivation strategy to improve electrocatalytic CO2 reduction reaction under aerobic conditions using a covalent organic frameworks with a photoswitching unit.
- Hong-Jing Zhu
- , Duan-Hui Si
- & Yuan-Biao Huang
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Article
| Open AccessFacilitating alkaline hydrogen evolution reaction on the hetero-interfaced Ru/RuO2 through Pt single atoms doping
Exploring an active and cost-effective catalyst for alkaline hydrogen evolution reaction remains elusive to date. Here, the authors report the platinum single-atoms doped ruthenium/ruthenium oxides showing distinctly enhanced catalytic performance.
- Yiming Zhu
- , Malte Klingenhof
- & Jiwei Ma
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Article
| Open AccessHigh-spin Co3+ in cobalt oxyhydroxide for efficient water oxidation
Regulating spin state of metal cations in catalysts is recognized as a strategy to improve water oxidation. Herein, the authors constructed high-spin cobalt ions in cobalt oxyhydroxides, experimentally demonstrating accelerated electron transfer ability and thereby superior water oxidation performance.
- Xin Zhang
- , Haoyin Zhong
- & Junmin Xue
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Article
| Open AccessIodide manipulation using zinc additives for efficient perovskite solar minimodules
Interstitial iodides are the most critical type of defects in perovskite solar cells that limits efficiency and stability. Here, the authors introduce small amount of zinc trifluoromethane sulfonate to control iodide defects, facilitating fabrication of minimodules with efficiencies of over 19%.
- Md Aslam Uddin
- , Prem Jyoti Singh Rana
- & Jinsong Huang
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Article
| Open AccessHierarchical Li electrochemistry using alloy-type anode for high-energy-density Li metal batteries
Utilizing an ultra-thin Li anode with a thickness below 50 μm is crucial for enhancing the energy density of batteries. Here, the authors develop a finely tunable, thin alloy-based Li anode that features a hierarchical Li electrochemistry, enabling stable cycling and superior energy density in Li metal batteries.
- Jiaqi Cao
- , Yuansheng Shi
- & Xia Lu
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Article
| Open AccessStructurally robust lithium-rich layered oxides for high-energy and long-lasting cathodes
O2-type Li-rich layered cathodes suppress voltage decay and aid in oxygen redox research. Here, the authors report trilateral relationship among anionic redox utilization, bulk chemo-mechanical degradation, and electrochemical fading, which can be mitigated by balancing the redox center capabilities.
- Ho-Young Jang
- , Donggun Eum
- & Kisuk Kang
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Article
| Open AccessEffect of sub-bandgap defects on radiative and non-radiative open-circuit voltage losses in perovskite solar cells
The efficiency of perovskite solar cells is affected by open-circuit voltage losses due to radiative and non-radiative charge recombination. Here, authors report photocurrent and electroluminescence spectroscopy to probe radiative recombination at sub-bandgap defects in wide-bandgap solar cells.
- Guus J. W. Aalbers
- , Tom P. A. van der Pol
- & René A. J. Janssen
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Article
| Open AccessSolvation-property relationship of lithium-sulphur battery electrolytes
In the Li-S battery, a promising next-generation battery chemistry, electrolytes are vital because of solvated polysulfide species. Here, the authors investigate solvation-property relationships via the measurement of solvation free energy of the electrolytes, guiding advanced electrolyte design for Li-S batteries.
- Sang Cheol Kim
- , Xin Gao
- & Yi Cui
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Article
| Open AccessRobust links in photoactive covalent organic frameworks enable effective photocatalytic reactions under harsh conditions
The development of heterogeneous photocatalysts applicable under harsh conditions is challenging. Here the authors report the conversion of imine linkages into quinoline groups in triphenylamine incorporated photosensitive covalent organic frameworks to develop robust heterogeneous photocatalysts for photocatalytic applications in harsh conditions.
- Jia-Rui Wang
- , Kepeng Song
- & Yanli Zhao
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Article
| Open AccessA nonmetallic plasmonic catalyst for photothermal CO2 flow conversion with high activity, selectivity and durability
In this work, the authors design a Mo2N/MoO2-x nonmetallic plasmonic catalyst by regulating synergy between two specific active sites. Highly efficient, selective, and durable CO2 hydrogenation under relatively mild reaction conditions is achieved
- Xueying Wan
- , Yifan Li
- & Yujie Xiong
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Article
| Open AccessRe-evaluation of battery-grade lithium purity toward sustainable batteries
Due to recent fluctuations in lithium prices, the instability of lithium-ion batteries prices is on the rise. Here, through a re-evaluation of purity criteria, the authors report that the presence of magnesium impurity in lithium precursor actually improves cathode performance, economics, and environmental aspects.
- Gogwon Choe
- , Hyungsub Kim
- & Yong-Tae Kim
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Article
| Open AccessRedox-tunable isoindigos for electrochemically mediated carbon capture
Electrochemically-mediated carbon capture has good energy efficiency and potential in carbon dioxide separation, but optimisation of these systems is challenging. Here, the authors report the use of isoindigo derivatives to give fine-tuned interactions with CO2 for carbon capture methods.
- Xing Li
- , Xunhua Zhao
- & Yayuan Liu
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Article
| Open AccessDecoupled oxidation process enabled by atomically dispersed copper electrodes for in-situ chemical water treatment
In-situ wastewater treatment using advanced oxidation processes poses ecological risks. Here, authors introduce a decoupled oxidation process with single-atom copper-based electrodes. This strategy overcomes drawbacks of AOPs, offering a sustainable and efficient in-situ treatment solution.
- Ziwei Yu
- , Xuming Jin
- & Juan Wang
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Article
| Open AccessTuning the apparent hydrogen binding energy to achieve high-performance Ni-based hydrogen oxidation reaction catalyst
Nickel-based electrocatalysts for the hydrogen oxidation reaction in hydroxide exchange membrane fuel cells show promise, but their activity requires further enhancement. Here, the authors report NiCuCr alloy with high activity, owing to the efficient tuning of both hydrogen and water binding on Ni sites by alloying with Cu and Cr.
- Xingdong Wang
- , Xuerui Liu
- & Zhongbin Zhuang
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Article
| Open AccessDesigning lithium halide solid electrolytes
The pursuit of all-solid-state batteries has motivated advancements in materials design. Here, the authors present a methodology demonstrating that ionic potential effectively captures crucial interactions within halide materials, guiding the design of the new materials with enhanced performance.
- Qidi Wang
- , Yunan Zhou
- & Marnix Wagemaker
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Article
| Open AccessSubtractive transformation of cathode materials in spent Li-ion batteries to a low-cobalt 5 V-class cathode material
Direct recycling or upcycling is promising for sustainable battery resource management. Here, the authors report a subtractive transformation strategy for upcycling spent cathode materials to high-performance 5 V-class cathodes, reducing reliance on rare elements for the sustainable Li-ion battery industry.
- Jun Ma
- , Junxiong Wang
- & Guangmin Zhou
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Article
| Open AccessSelf-assembled hydrated copper coordination compounds as ionic conductors for room temperature solid-state batteries
The design of inorganic-organic hybrid solid-state electrolytes is expected to merge the merits of both inorganic and organic material. Here, the authors craft Li-ion-implanted copper maleate hydrate nanoflakes via a bottom-up self-assembly approach to reveal superior room-temperature Li-ion conductivity.
- Xiao Zhan
- , Miao Li
- & Li Zhang