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| Open AccessA scalable Li-Al-Cl stratified structure for stable all-solid-state lithium metal batteries
Sulfide electrolytes’ incompatibility with Li metal hinders their use in all-solid-state Li metal batteries. Here, the authors propose a scalable Li-Al-Cl stratified structure, formed via strain-activated phase separation, to effectively stabilize the negative electrode/electrolyte interface.
- Han Su
- , Jingru Li
- & Jiangping Tu
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Article
| Open AccessPolymer hetero-electrolyte enabled solid-state 2.4-V Zn/Li hybrid batteries
Zn batteries suffer from low voltage due to the high redox potential of the Zn anode and the low potential of traditional cathodes. Here, the authors develop a polymer hetero-electrolyte, which allows separated Zn and Li reversibility and achieves a 2.4 V-Zn battery based on the LiNi0.5Mn1.5O4 cathode.
- Ze Chen
- , Tairan Wang
- & Chunyi Zhi
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Article
| Open AccessCatalytic role of in-situ formed C-N species for enhanced Li2CO3 decomposition
Sluggish kinetics of the CO2 reactions lead to the accumulation of Li2CO3 residuals, which hinders the cycling stability of Li-CO2 batteries. Here, the authors reveal the catalytic role of in-situ formed C-N species in enhancing the reversibility of Li2CO3 and cycle life of Li-CO2 batteries.
- Fangli Zhang
- , Wenchao Zhang
- & Zaiping Guo
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Article
| Open AccessSurface oxidation/spin state determines oxygen evolution reaction activity of cobalt-based catalysts in acidic environment
Co-based catalysts are promising candidates for oxygen evolution reaction catalysis in an acidic environment, but the structure-activity relationship is unclear. Here, the authors discover that their acidic water oxidation activity is determined by the surface oxidation/spin state.
- Jinzhen Huang
- , Camelia Nicoleta Borca
- & Emiliana Fabbri
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| Open AccessExciton engineering of 2D Ruddlesden–Popper perovskites by synergistically tuning the intra and interlayer structures
Guo et al. report enhanced emission and photoconductivity in 2D Ruddlesden-Popper perovskites by synergistically tuning the intra and interlayer structure via pressure. A structure descriptor considering both intra- and interlayer is then introduced for screening perovskite with desired properties.
- Songhao Guo
- , Willa Mihalyi-Koch
- & Xujie Lü
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Article
| Open AccessA silicon photoanode protected with TiO2/stainless steel bilayer stack for solar seawater splitting
Here, the authors report a Si photoanode coated with a TiO2/stainless steel bilayer to inhibit chloride adsorption and facilitate stable alkaline seawater splitting for over 50 h with an applied bias photon-to-current efficiency of 2.62%.
- Shixuan Zhao
- , Bin Liu
- & Jinlong Gong
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Article
| Open AccessAluminum corrosion–passivation regulation prolongs aqueous batteries life
Aqueous batteries have a short lifespan due to Al current collector corrosion and Li loss from side reactions on the anode. Here, the authors propose a prototype of self-prolonging aqueous Li-ion batteries by introducing hydrolyzation-type anodic additives to regulate Al corrosion-passivation.
- Binghang Liu
- , Tianshi Lv
- & Liumin Suo
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Article
| Open AccessIsotope engineering achieved by local coordination design in Ti-Pd co-doped ZrCo-based alloys
Hydrogen isotope effect in metal-hydrogen systems disturbs precise Deuterium/Tritium (D/T) ratio control. Here, the authors demonstrate a local coordination strategy that comprises thermodynamic destabilization with vibration enhancement of interstitial isotopes for isotope engineering.
- Jiacheng Qi
- , Xu Huang
- & Lixin Chen
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Article
| Open AccessEnhancement of electrocatalysis through magnetic field effects on mass transport
Magnetic fields can enhance electrocatalysis, yet its effect on mass transport has been overlooked. Here, the authors track the motion induced on the electrolyte ions, demonstrating that mass transport effects can double the catalyst activity with low reactant availability, as in oxygen reduction.
- Priscila Vensaus
- , Yunchang Liang
- & Magalí Lingenfelder
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Article
| Open AccessAn integrated high-throughput robotic platform and active learning approach for accelerated discovery of optimal electrolyte formulations
Solubility determines energy density in redox flow batteries. Here, authors combine automated experiments with machine learning to efficiently identify solvents that significantly enhance solubility, testing less than 10% of over 2000 candidates.
- Juran Noh
- , Hieu A. Doan
- & Yangang Liang
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Article
| Open AccessUnderstanding the effect of spatially separated Cu and acid sites in zeolite catalysts on oxidation of methane
Methane is a potent greenhouse gas, and its removal is critical. Here, the authors demonstrate that spatially separated Cu and acid sites in Cu/zeolites influence product distribution and efficiency for methane oxidation.
- Peipei Xiao
- , Yong Wang
- & Toshiyuki Yokoi
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Article
| Open AccessUltra-fast green hydrogen production from municipal wastewater by an integrated forward osmosis-alkaline water electrolysis system
Green hydrogen production faces increased water risks due to scarce supplies of water. Here, authors develop a modular forward osmosis-water splitting system that utilises wastewater effluent to generate high-purity hydrogen, providing a sustainable solution for water and energy security.
- Gabriela Scheibel Cassol
- , Chii Shang
- & Li Ling
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Article
| Open AccessDeciphering the critical role of interstitial volume in glassy sulfide superionic conductors
Glass sulfide electrolytes are promising materials for solid-state Li metal batteries, yet limited understanding hinders their progress. Here, the authors decipher the dissolution process of halogen dopants in glass and introduce a synthetic strategy to increase halogen dopant’s dissolution capacity.
- Han Su
- , Yu Zhong
- & Jiangping Tu
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Article
| Open AccessSingle-atom platinum with asymmetric coordination environment on fully conjugated covalent organic framework for efficient electrocatalysis
In addition to maximizing atomic utilization, single-atom catalysts with defined structures can be used to investigate catalytic mechanisms and structure-activity relationships. Here, authors study a non-thermodynamically stable Pt-N2 active site for the electrochemical hydrogen evolution reaction.
- Ziqi Zhang
- , Zhe Zhang
- & Shouhua Feng
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Article
| Open AccessWell-defined diatomic catalysis for photosynthesis of C2H4 from CO2
Principal interest lies in diatomic catalysts (DACs) for efficient CO2 to C2H4 photoconversion yet optimizing catalytic performance and exploring reaction mechanisms are impeded by heteronuclear atom random distribution. Here, a novel up-bottom ion-cutting architecture is proposed for fabricating well-defined DACs.
- Zhongkai Xie
- , Shengjie Xu
- & Shuyan Song
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Article
| Open AccessSelenium substitution for dielectric constant improvement and hole-transfer acceleration in non-fullerene organic solar cells
Dielectric constant of non-fullerene acceptors plays a critical role in organic solar cells in terms of exciton dissociation and charge recombination. Here, authors report selenium substitution on central core of acceptors to improve dielectric constant, realizing devices with efficiency of 19.0%.
- Xinjun He
- , Feng Qi
- & Wallace C. H. Choy
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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 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 AccessNanocurvature-induced field effects enable control over the activity of single-atom electrocatalysts
Modulating interfacial electric fields provides a means to control electrocatalyst activity for a broad range of reactions. Here the authors show that this can be achieved by tuning the nanocurvature of carbon supported single-atom catalysts.
- Bingqing Wang
- , Meng Wang
- & Yanwei Lum
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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 AccessDecoupled electrolysis for hydrogen production and hydrazine oxidation via high-capacity and stable pre-protonated vanadium hexacyanoferrate
Decoupled electrolysis with the aid of a redox mediator offers great flexibility in operation. Here, the authors construct a decoupled electrolysis system for separate hydrogen production and electricity generation to achieve flexible energy conversion and storage using renewables.
- Fei Lv
- , Jiazhe Wu
- & Yubin Chen
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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 AccessAcidic media enables oxygen-tolerant electrosynthesis of multicarbon products from simulated flue gas
Direct electroreduction of dilute CO2 in flue gas streams is challenging due to the presence of O2 impurities. Here the authors demonstrate that an acidic electrolyte can overcome this challenge, enabling the generation of multicarbon products from simulated flue gas at reasonable rates.
- Meng Wang
- , Bingqing Wang
- & Yanwei Lum
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Article
| Open AccessHigh voltage electrolytes for lithium-ion batteries with micro-sized silicon anodes
Micro-sized silicon are promising anode materials due to low-cost and high-energy, yet their application is hindered by inaccessible electrolytes. Here, the authors report sulfolane-based electrolytes that form silicon-phobic interphases and enable high-voltage pouch cells to achieve superior cycle life.
- Ai-Min Li
- , Zeyi Wang
- & Chunsheng 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 AccessA rechargeable Ca/Cl2 battery
The development of practical Ca metal batteries has been hindered by the cathode chemistry. Here, the authors report a rechargeable Ca/Cl2 battery, which involves the reversible cathode redox reaction between CaCl2 and Cl2.
- Shitao Geng
- , Xiaoju Zhao
- & Hao Sun
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Article
| Open AccessHomolytic H2 dissociation for enhanced hydrogenation catalysis on oxides
Zhu et al. report a quantitative and time-resolved analysis of hydrogen activation on Ga2O3, specifically shedding light on the long-standing puzzle of homolytic dissociation as opposed to the heterolytic pathway on oxides.
- Chengsheng Yang
- , Sicong Ma
- & Xinhe Bao
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Article
| Open AccessEfficient and stable visible-light-driven Z-scheme overall water splitting using an oxysulfide H2 evolution photocatalyst
Photocatalytic water splitting systems using Sm2Ti2O5S2, a visible light-active oxysulfide, exhibited low efficiencies due to low intrinsic photoactivity and rapid back reaction. Here, the efficiency was greatly improved by refining the preparation of photocatalysts and electron mediators
- Lihua Lin
- , Yiwen Ma
- & Kazunari Domen
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Article
| Open AccessUniversal machine learning aided synthesis approach of two-dimensional perovskites in a typical laboratory
Chemical synthesis of advanced functional materials remains a complex and multidimensional challenge. Here, authors develop a data-driven framework to increase the success rate of the synthesis of two-dimensional perovskites.
- Yilei Wu
- , Chang-Feng Wang
- & Jinlan Wang
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Article
| Open AccessGiant adiabatic temperature change and its direct measurement of a barocaloric effect in a charge-transfer solid
Cyano-RbMnFeCo shows a large barocaloric effect with reversible adiabatic temperature changes of 74 K (340 MPa) and 85 K (560 MPa). Here, the authors observe temperature change of +44 K (440 MPa), stable after repeating over 100 times.
- Shin-ichi Ohkoshi
- , Kosuke Nakagawa
- & Ryu Hatano
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Article
| Open AccessSintering-induced cation displacement in protonic ceramics and way for its suppression
The conductivity of protonic ceramic electrolytes for fuel cells is unsatisfactory due to poor sintering. Here, the authors report the adverse effects of dynamic Y3+ displacement on high-temperature membrane sintering and propose a new strategy for pre-doping Y into A-site to inhibit its further displacement.
- Ze Liu
- , Yufei Song
- & Linjuan Zhang
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Article
| Open AccessDesigning Cu0−Cu+ dual sites for improved C−H bond fracture towards methanol steam reforming
Cu-based catalysts are widely considered to be effective materials for H2 production via methanol steam reforming. Herein, the authors explore a series of catalysts containing Cu0−Cu+ dual sites for facilitating C-H bond breaking and H2 evolution.
- Hao Meng
- , Yusen Yang
- & Min Wei
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Article
| Open AccessNonredox trivalent nickel catalyzing nucleophilic electrooxidation of organics
A good understanding of the mechanism behind organic electrooxidation is crucial for the development of efficient energy conversion technology. Here, the authors find that trivalent nickel is capable of oxidizing organics through a nucleophilic attack and electron transfer via a non-redox process.
- Yuandong Yan
- , Ruyi Wang
- & Zhigang Zou
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Article
| Open AccessA promising perovskite primary explosive
A primary explosive (DPPE-1) with a double perovskite structure and ignition function was reported. It is synthesized in a straightforward manner and has good stability, with a minimum primary charge of 5 mg.
- Yongan Feng
- , Jichuan Zhang
- & Jean’ne M. Shreeve
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Article
| Open AccessHigh proton conductivity within the ‘Norby gap’ by stabilizing a perovskite with disordered intrinsic oxygen vacancies
Proton conductors are promising materials used in various applications such as fuel cells. Here, authors report high proton conductivity due to the reduction of proton trapping of donor Mo6+ doped BaScO2.5 with disordered intrinsic oxygen vacancies.
- Kei Saito
- & Masatomo Yashima
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Article
| Open AccessImproving the photovoltage of Cu2O photocathodes with dual buffer layers
Increasing the photovoltage of the Cu2O photocathode plays an important role in photocatalytic water splitting. Here the authors construct a dual buffer layer to optimize the band alignment between the n-type layer and the protective layer, which improves the onset potential of the Cu2O photocathode by 0.16 V.
- Jinshui Cheng
- , Linxiao Wu
- & Jingshan Luo
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Article
| Open AccessImprovement of oxygen reduction activity and stability on a perovskite oxide surface by electrochemical potential
Solid oxide fuel and electrolysis cells suffer from surface instability which challenges their performance and durability. Here, the authors report that cathodic polarization improves the electrochemical activity by formation of Ruddlesden-Popper phase, exsolution of Co, and suppression of Sr segregation.
- Sanaz Koohfar
- , Masoud Ghasemi
- & Bilge Yildiz
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Article
| Open AccessMetal-free photoanodes for C–H functionalization
The photoelectrochemical performance of carbon nitride is still insufficient for organic transformations. Here, the authors introduce a spin coating strategy for the synthesis of carbon nitride photoelectrodes, enabling high yields in C-H functionalization.
- Junfang Zhang
- , Yuntao Zhu
- & Felix F. Loeffler
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Article
| Open AccessIntercalation-type catalyst for non-aqueous room temperature sodium-sulfur batteries
Sodium-sulfur batteries show potential as attractive alternatives to Li-ion batteries due to their high energy density but practicality is hampered by sodium polysulfide issues. Here, the authors introduce an intercalation-type catalyst MoTe2 to improve the redox kinetics in Na-S batteries.
- Jiarui He
- , Amruth Bhargav
- & Arumugam Manthiram
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Article
| Open AccessElectrochemically induced crystalline-to-amorphization transformation in sodium samarium silicate solid electrolyte for long-lasting sodium metal batteries
Solid-state sodium metal batteries require solid electrolytes with high ionic conductivity and optimal electrode compatibility. Here, the authors introduce the Na5SmSi4O12 solid electrolyte with a crystalline-to-amorphous transformation, achieving 4000 cycles lifetime without capacity decline.
- Ge Sun
- , Chenjie Lou
- & Fei Du
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Article
| Open AccessPhase regulation enabling dense polymer-based composite electrolytes for solid-state lithium metal batteries
Polymer electrolytes based on poly(vinylidene fluoride) with residual solvents are appealing for room-temperature battery operations. Here, the authors present a phase regulation approach to achieve a dense electrolyte and enhance ionic conductivity through the incorporation of MoSe2 sheets.
- Qian Wu
- , Mandi Fang
- & Yingying Lu
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Article
| Open AccessMetal to non-metal sites of metallic sulfides switching products from CO to CH4 for photocatalytic CO2 reduction
The product selectivity of photocatalytic carbon dioxide reduction from carbon monoxide to methane is determined by the active center from metal to sulfur site in metal sulfides. Non-metal sulfur in CuInSnS4 octahedral nanocrystal acts as carbon dioxide activation center for switching selectivity to methane.
- Yao Chai
- , Yuehua Kong
- & Zizhong Zhang
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Article
| Open AccessLow-temperature anode-free potassium metal batteries
Low temperature operation of anode-free batteries is limited by poor reversibility of metal plating/stripping. Here, via electrolyte engineering, authors enable −40 °C operation of an anode-free K metal battery by tailoring a weakly solvating electrolyte with a silicone polymer additive.
- Mengyao Tang
- , Shuai Dong
- & Hua Wang
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Article
| Open AccessBoosting urea electrooxidation on oxyanion-engineered nickel sites via inhibited water oxidation
Urea electrooxidation reaction is of great importance in energy related applications and devices but is limited by competing oxygen evolution reaction. Here, the authors report oxyanion-engineered nickel catalysts that can achieve efficient urea oxidation while suppressing oxygen evolution reaction.
- Xintong Gao
- , Xiaowan Bai
- & Shi-Zhang Qiao
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Article
| Open AccessInterfacial friction enabling ≤ 20 μm thin free-standing lithium strips for lithium metal batteries
Thin, freestanding Li metal foils are key to improving the energy density of Li batteries but are difficult to manufacture. Here, authors achieve thin Li foils by mechanical rolling, exploiting tribochemistry to form a protective surface film that improves mechanical and electrochemical properties.
- Shaozhen Huang
- , Zhibin Wu
- & Libao Chen
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Article
| Open AccessSelective CO2 reduction to CH3OH over atomic dual-metal sites embedded in a metal-organic framework with high-energy radiation
Most approaches for CH3OH production focus on thermochemical, electrolytic, and photolytic processes. Here the authors report a radiolytic route to produce CH3OH from CO2 and water by atomic Cu-Ni dual sites embedded in a metal-organic framework.
- Changjiang Hu
- , Zhiwen Jiang
- & Jun Ma
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Article
| Open AccessElectro-assisted methane oxidation to formic acid via in-situ cathodically generated H2O2 under ambient conditions
This study presents the electrochemically assisted partial oxidation of methane to produce liquid oxygenate, HCOOH, selectively which involves in-situ cathodically generated reactive oxygen species with an acid-treated carbon electrocatalyst.
- Jiwon Kim
- , Jae Hyung Kim
- & Yun Jeong Hwang
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Article
| Open AccessA rare case of brominated small molecule acceptors for high-efficiency organic solar cells
The relatively larger steric hindrance and excessive crystallinity of bromides could lead to undesirable film morphologies. Here, the authors take advantage of bromides and construct small molecule acceptors with stepwise bromination and realize maximum efficiency of 19% in organic solar cells.
- Huazhe Liang
- , Xingqi Bi
- & Yongsheng Chen
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Article
| Open AccessReaction-passivation mechanism driven materials separation for recycling of spent lithium-ion batteries
Separating active cathode materials from current collectors poses a critical challenge in battery recycling. Here, the authors develop a facile strategy that relies on a reaction-passivation mechanism to effectively separate the aluminum foil and cathode active material in spent lithium-ion batteries.
- Zihe Chen
- , Ruikang Feng
- & Yongming Sun