Featured
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| 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
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Article
| Open AccessExperimental manifestation of redox-conductivity in metal-organic frameworks and its implication for semiconductor/insulator switching
MOFs that transport electrons by a hopping mechanism are redox conductors. Here authors demonstrate a diagnostic bell-shaped conductivity curve that is centred around the formal potential of the redox active unit in a variety of MOFs.
- Jingguo Li
- , Amol Kumar
- & Sascha Ott
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Article
| Open AccessProduction of gas-releasing electrolyte-replenishing Ah-scale zinc metal pouch cells with aqueous gel electrolyte
The production of large-format aqueous Zn batteries is hindered by electrolyte consumption, hydrogen gas evolution and Zn dendrites growth during cycling. Here, the authors propose a specific pouch cell design capable of releasing hydrogen gas and refilling the electrolyte components.
- Feifei Wang
- , Jipeng Zhang
- & Quan-Hong Yang
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Article
| Open AccessAcidic enol electrooxidation-coupled hydrogen production with ampere-level current density
Hydrogen production coupled with biomass upgrading is vital for sustainable energy developments. Here, the authors report an acidic hydrogen production system that combines enol electrooxidation to achieve industrial current densities with an operating bias of less than 1.23 V.
- Zheng-Jie Chen
- , Jiuyi Dong
- & Hui-Ming Cheng
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Article
| Open AccessAsymmetric gradient orbital interaction of hetero-diatomic active sites for promoting C − C coupling
Molecular insights into the selectivity mechanism of dual-atom sites are required to engineer efficient solar-fuel catalysts. Here, the authors reveal symmetry-forbidden coupling mechanism of C1 intermediates on diatomic sites by manipulating metal gradient orbital interaction over diatomic COFs.
- Jin Ming Wang
- , Qin Yao Zhu
- & Tae Kyu Kim
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Article
| Open AccessA cost-effective, ionically conductive and compressible oxychloride solid-state electrolyte for stable all-solid-state lithium-based batteries
Ionic conductivity > 1 mS cm−1 at 25 °C, compressibility enabling > 90% density at 250 − 350 MPa, and cost < $50/kg are desirable for inorganic solid-state electrolytes. Here, the authors report Li1.75ZrCl4.75O0.5 as a solid-state electrolyte capable of satisfying these requirements simultaneously.
- Lv Hu
- , Jinzhu Wang
- & Cheng Ma
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Article
| Open AccessPost-synthetic modification of covalent organic frameworks for CO2 electroreduction
Covalent organic frameworks constructed with ionic skeletons and C-N linkages by multilevel post-synthetic modification. These frameworks achieved high activity and stability for electrocatalytic CO2 reduction.
- Minghao Liu
- , Shuai Yang
- & Gaofeng Zeng
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Article
| Open AccessBridging multiscale interfaces for developing ionically conductive high-voltage iron sulfate-containing sodium-based battery positive electrodes
Sluggish kinetics is a major challenge for iron-based sulfate electrode materials. Here, the authors report multiscale interface engineering to build continuous Na-ion transfer channels at all length scales by designing ionic conductors inside bulk and low-electron-density exposed crystal surfaces.
- Jiyu Zhang
- , Yongliang Yan
- & Weihua Chen
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Article
| Open AccessDissolved-Cl2 triggered redox reaction enables high-performance perovskite solar cells
Constructing 2D/3D perovskite heterojunctions is effective for the surface passivation of perovskite solar cells. Here, the authors apply Cl2-dissolved chloroform as a multifunctional solvent and achieve a champion device efficiency of 24.21% with improved thermal, ambient and operational stability.
- Yujie Luo
- , Kaikai Liu
- & Zhanhua Wei
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Article
| Open AccessProduction of high-energy 6-Ah-level Li | |LiNi0.83Co0.11Mn0.06O2 multi-layer pouch cells via negative electrode protective layer coating strategy
Stable lithium metal electrodes are needed to produce high-energy batteries. Here, authors reported poly(2-hydroxyethyl acrylate-co-sodium benzenesulfonate) as a lithium metal protective layer and the production of a 490 Wh/kg class Li | |LiNi0.83Co0.11Mn0.06O2 pouch cell.
- Yangyang Feng
- , Yong Li
- & Yaobing Wang
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Article
| Open AccessA corrosion-resistant RuMoNi catalyst for efficient and long-lasting seawater oxidation and anion exchange membrane electrolyzer
Direct seawater electrolysis is promising for sustainable hydrogen production but suffers severe side reactions and corrosion. Here, the authors report a corrosion-resistant electrocatalyst with in situ-formed chloride-ion-repelling cation layer for efficient and long-lasting seawater oxidation.
- Xin Kang
- , Fengning Yang
- & Bilu Liu
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Article
| Open AccessEnabling long-cycling aqueous sodium-ion batteries via Mn dissolution inhibition using sodium ferrocyanide electrolyte additive
Mn-based Prussian blue is an ideal positive electrode material for aqueous sodium-ion batteries but still suffers from Mn dissolution. Here, the authors introduce an Mn-ion trapping agent as an electrolyte additive to produce a 94 Wh kg−1 Na-ion aqueous battery with a long lifespan.
- Zhaoheng Liang
- , Fei Tian
- & Chengxin Wang