Featured
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| 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
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Article
| Open AccessAccelerating the solar-thermal energy storage via inner-light supplying with optical waveguide
Phase change material for solar-thermal energy storage is widely studied to counter the mismatch between supply and demand in solar energy utilization. Here, authors introduce optical waveguide to regulate the solar-thermal conversion interface to enable the fast energy harvesting in solar-thermal energy storage system.
- Yafang Zhang
- , Jiebin Tang
- & Guobin Xue
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Article
| Open AccessSingle-site decorated copper enables energy- and carbon-efficient CO2 methanation in acidic conditions
Conventional alkaline and neutral CO2-to-CH4 systems suffer carbon loss, and recovering the lost carbon requires input energy exceeding the heating value of CH4. Here, the authors report a chelating strategy to obtain Cu-N/O single sites decorated Cu clusters, which enables energy- and carbon-efficient CH4 electroproduction in an acidic system.
- Mengyang Fan
- , Rui Kai Miao
- & David Sinton
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Article
| Open AccessExtreme fast charging of commercial Li-ion batteries via combined thermal switching and self-heating approaches
A significant barrier to the mass adoption of electric vehicles is the long charge time (>30 min) of high-energy Li-ion batteries. Here, the authors propose a practical solution to enable fast charging of commercial Li-ion batteries by combining thermal switching and self-heating.
- Yuqiang Zeng
- , Buyi Zhang
- & Ravi S. Prasher
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Article
| Open AccessBioinspired design of Na-ion conduction channels in covalent organic frameworks for quasi-solid-state sodium batteries
Quasi-solid-state polymer electrolytes are ideal candidates for practical secondary battery applications. Here, the authors propose a negatively charged (–COO–)-modified covalent organic framework as a Na-ion quasi-solid-state electrolyte with sub-nanometric Na-ion transport zones.
- Yingchun Yan
- , Zheng Liu
- & Zhuangjun Fan
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Article
| Open AccessSurface plasmon-enhanced photo-driven CO2 hydrogenation by hydroxy-terminated nickel nitride nanosheets
Plasmonic catalysts are often limited to Au, Ag, Cu, Al, etc. Now, hydroxy-terminated nickel nitride nanosheets are reported to be an alternative material for CO2 hydrogenation to CO using solar energy without co-catalysts or sacrificial agents.
- Saideep Singh
- , Rishi Verma
- & Vivek Polshettiwar
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Article
| Open AccessPhotocatalytic CO2 reduction using La-Ni bimetallic sites within a covalent organic framework
A bifunctional dual-atom photocatalysts with La and Ni sites is shown to be have efficient generation and transfer of photocarriers from the optically active La center to the catalytically active Ni center for promoting efficient CO2 reduction to CO.
- Min Zhou
- , Zhiqing Wang
- & Yueli Liu
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Article
| Open AccessBoosting the interfacial superionic conduction of halide solid electrolytes for all-solid-state batteries
Compositional tuning is a standard procedure to improve the ionic conductivity of inorganic superionic conductors. Here, the authors report (electro)chemical stable composite halide solid electrolytes applying a nanostructure approach that promotes interfacial superionic conductivity.
- Hiram Kwak
- , Jae-Seung Kim
- & Yoon Seok Jung
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Article
| Open AccessEffect of pulse-current-based protocols on the lithium dendrite formation and evolution in all-solid-state batteries
The practical use of all-solid-state batteries is hindered by lithium dendrites formed at current densities lower than the threshold suggested by industry research. Here, the authors propose a MHz-pulse-current protocol to circumvent the low-current cell failure and provide mechanistic analyses.
- V. Reisecker
- , F. Flatscher
- & D. Rettenwander
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Article
| Open AccessA high-temperature double perovskite molecule-based antiferroelectric with excellent anti-breakdown capacity for energy storage
Antiferroelectric (AFE) materials are emerging as a remarkable candidate for efficient energy-storage applications. Here, the authors report on a high-temperature, lead-free, AFE perovskite, (CHMA)2CsAgBiBr7 (where CHMA is cyclohexylmethylammonium) with high fatigue endurance at a high electric breakdown field strength.
- Yi Liu
- , Yu Ma
- & Zhihua Sun
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Article
| Open AccessInsights into solvent and surface charge effects on Volmer step kinetics on Pt (111)
Excess free charges on electrode surfaces drive changes in hydrogen electrocatalysis kinetics. Here, the authors show how redox solvent reorganization energy is insensitive to interfacial electric field strength; instead, the charged surface directly modulates proton electrochemical potential.
- Jon C. Wilson
- , Stavros Caratzoulas
- & Yushan Yan
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Article
| Open AccessAlgal cell bionics as a step towards photosynthesis-independent hydrogen production
Low rate and limited duration are major challenges in photobiological hydrogen production. Here, the authors coat algal cells with a concentrically arranged shell comprising an ultra-thin Fe(III)-doped polypyrrole inner layer and outer exoskeleton of CaCO3, and achieve sustainable H2 production for over 200 days.
- Zhijun Xu
- , Jiarui Qi
- & Xin Huang
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Article
| Open AccessInterfacial assembly of binary atomic metal-Nx sites for high-performance energy devices
An interfacial assembly strategy was developed to construct single-atom binary Fe/Co-Nx sites with a high accessible site density of 7.6 × 1019 sites per gram which results in increased power densities in fuel cells and Zn/air batteries.
- Zhe Jiang
- , Xuerui Liu
- & Jin-Song Hu
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Article
| Open AccessSulfolane-containing aqueous electrolyte solutions for producing efficient ampere-hour-level zinc metal battery pouch cells
The negative electrode reversibility limits the lifespan of Zn metal batteries. Here, authors report an aqueous electrolyte with a reverse micelle structure that improves the reversibility of the Zn metal anode enabling the production of an ampere-hour-level pouch cell with five months lifetime.
- Yu Wang
- , Tairan Wang
- & Chunyi Zhi
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Article
| Open AccessImproving CO2 photoconversion with ionic liquid and Co single atoms
There is growing interest in designing photocatalysts for CO2 conversion. Here, the authors combine an ionic liquid with Co single atoms as dual-cocatalysts for g-C3N4, accelerating electron kinetics and improving CO2 reduction selectivity.
- Yang Liu
- , Jianhui Sun
- & Liqiang Jing
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Article
| Open AccessNanoarchitecture factors of solid electrolyte interphase formation via 3D nano-rheology microscopy and surface force-distance spectroscopy
Characterization of the solid electrolyte interphase formed on Li-ion battery electrodes presents significant experimental challenges. Here the authors use atomic force microscopy-based force-spectroscopy techniques to depict the initial interphase formation in two different electrolyte classes.
- Yue Chen
- , Wenkai Wu
- & Oleg V. Kolosov
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Article
| Open AccessLigand vacancy channels in pillared inorganic-organic hybrids for electrocatalytic organic oxidation with enzyme-like activities
Undercoordinated metal sites with well-defined structures and stability are desired properties for catalysts. Here, the authors construct a class of inorganic-organic hybrid electrocatalysts with enzyme-like properties, which exhibit enhanced electrochemical oxidation of 25 different organics.
- Zhe Chen
- , Jili Li
- & Ming Gong
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Article
| Open AccessA monofluoride ether-based electrolyte solution for fast-charging and low-temperature non-aqueous lithium metal batteries
The energy content of non-aqueous lithium batteries is limited by the electrochemical stability window of the electrolyte solution. Here, the authors report a monofluoride ether-based electrolyte to stabilize high-voltage lithium metal batteries at high current rates and low temperatures.
- Guangzhao Zhang
- , Jian Chang
- & Jun Lu
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Article
| Open AccessPhotocatalytic CO2 reduction with aminoanthraquinone organic dyes
A class of inexpensive aminoanthraquinone organic dyes are shown to facilitate visible-light-driven CO2 reduction. Overall reaction efficiencies were found to be optimal when both electron donating and accepting groups were on a single dye molecule.
- Qinqin Lei
- , Huiqing Yuan
- & Zhiji Han
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Article
| Open AccessElectrolyte design principles for developing quasi-solid-state rechargeable halide-ion batteries
State-of-the-art electrolytes limit the cycle life of halide-ion batteries. Here, the authors report a fluorinated low-polar gel polymer electrolyte capable of improving the stability of the electrolyte and electrode interphases to boost battery performance.
- Xu Yang
- , Bao Zhang
- & Guoxiu Wang
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Article
| Open AccessNon-polar ether-based electrolyte solutions for stable high-voltage non-aqueous lithium metal batteries
Ether solvents have poor anodic stabilities in lithium metal batteries. Here, the authors propose a non-aqueous electrolyte solution with a non-polar and non-fluorinated ether solvent. The electrolyte enables stable cycling of high-voltage Li metal batteries in pouch cell configuration.
- Zheng Li
- , Harsha Rao
- & Vilas G. Pol
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Article
| Open AccessSurface engineering of inorganic solid-state electrolytes via interlayers strategy for developing long-cycling quasi-all-solid-state lithium batteries
Lithium metal batteries (LMBs) with inorganic solid-state electrolytes suffer from lithium dendrites propagation. Here, the authors demonstrate the production of stable lab-scale LMBs using an Ag-coated Li6.4La3Zr1.7Ta0.3O12 inorganic solid electrolyte in combination with a silver-carbon interlayer.
- Ju-Sik Kim
- , Gabin Yoon
- & Dongmin Im
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Article
| Open AccessA hydrophobic Cu/Cu2O sheet catalyst for selective electroreduction of CO to ethanol
Tuning electrocatalytic reduction of carbon monoxide to achieve valuable ethanol product with high performance is interesting yet challenging. Here, the authors design a hydrophobic Cu/Cu2O sheet catalyst showing a FE of 68.8% and partial current density of 111 mA cm−2 for CO reduction to ethanol.
- Guifeng Ma
- , Olga A. Syzgantseva
- & Buxing Han
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Article
| Open AccessCOx hydrogenation to methanol and other hydrocarbons under mild conditions with Mo3S4@ZSM-5
A series of materials containing Mo-S clusters confined in zeolitic cages of ZSM-5 are reported and shown to be efficient for CO2 or CO hydrogenation with >98% selectivity to methanol, stable over 1000 h, or C2 and C3 hydrocarbons, stable over 100 h.
- Gui Liu
- , Pengfei Liu
- & Weiping Ding
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Perspective
| Open AccessA non-academic perspective on the future of lithium-based batteries
In the field of lithium-based batteries, there is often a divide between academic research and industrial needs. Here, the authors present a view on applied research to help bridge academia and industry, focusing on metrics and challenges to be considered for the development of practical batteries.
- James T. Frith
- , Matthew J. Lacey
- & Ulderico Ulissi
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Article
| Open AccessDynamic rhenium dopant boosts ruthenium oxide for durable oxygen evolution
RuO2 is a promising anode catalyst for proton exchange membrane water electrolyzers but suffers from poor catalytic stability. Here the authors present a rhenium-doped RuO2 with a unique dynamic electron accepting-donating that adaptively boosts activity and stability in acidic water oxidation.
- Huanyu Jin
- , Xinyan Liu
- & Shi-Zhang Qiao
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Article
| Open AccessBottom-up evolution of perovskite clusters into high-activity rhodium nanoparticles toward alkaline hydrogen evolution
Self-reconstruction is an efficient method to synthesize active electrocatalysts. Here, the authors demonstrate a bottom-up evolution route of electrochemically reducing Cs3Rh2I9 halide-perovskite clusters to prepare ultrafine Rh nanoparticles with multiply sites for alkaline hydrogen evolution.
- Gaoxin Lin
- , Zhuang Zhang
- & Jiacheng Wang
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Article
| Open AccessPt nanoclusters on GaN nanowires for solar-asssisted seawater hydrogen evolution
Seawater is the most abundant water source for hydrogen fuel production. Here the authors report a binary photoelectrode of Pt catalyst-GaN semiconductor with promising efficiency, productivity, and stability for seawater hydrogen evolution.
- Wan Jae Dong
- , Yixin Xiao
- & Zetian Mi
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Article
| Open AccessA gradient oxy-thiophosphate-coated Ni-rich layered oxide cathode for stable all-solid-state Li-ion batteries
Layered oxide cathode active materials suffer from interfacial structural instability when coupled with sulfide solid-state electrolytes. Here, the authors propose a gradient coating with a lithium oxythiophosphate layer that can stabilize the cathode|solid-state electrolyte interface.
- Jianwen Liang
- , Yuanmin Zhu
- & Xueliang Sun
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Article
| Open AccessAuto-accelerated dehydrogenation of alkane assisted by in-situ formed olefins over boron nitride under aerobic conditions
Oxidative dehydrogenation of alkanes over boron nitride catalysts provides a new opportunity for efficient olefin production. Here, the authors discover in situ formed olefins can promote parent alkane conversion, and achieve activation of ethane by propane-derived olefins at a lower temperature.
- Zhankai Liu
- , Ziyi Liu
- & An-Hui Lu
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Article
| Open AccessConstructing robust heterostructured interface for anode-free zinc batteries with ultrahigh capacities
The development of dendrite-free, Zn-free anodes is challenging. Here, the authors design a two-dimensional antimony/antimony-zinc alloy heterostructured interface to achieve dendrite-free Zn deposition with areal capacity of 200 mAh cm−2, and energy density of around 270 Wh kg−1 for anode-free zinc-bromine battery.
- Xinhua Zheng
- , Zaichun Liu
- & Wei Chen
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Article
| Open AccessDual fluorination of polymer electrolyte and conversion-type cathode for high-capacity all-solid-state lithium metal batteries
The practical use of all-solid-state batteries is hindered by inadequate cycling performance. Here, the authors propose a fluorination strategy for the positive electrode and polymeric electrolyte to develop all-solid-state Li||FeF3 pouch cells with high discharge capacity and long cycle life.
- Jiulin Hu
- , Chuanzhong Lai
- & Chilin Li
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Article
| Open AccessUnlocking the hidden chemical space in cubic-phase garnet solid electrolyte for efficient quasi-all-solid-state lithium batteries
Conventional compositions of garnet solid electrolytes have limited access to the cubic phase for a high Li content of 7.0, which is beneficial for stability against Li metals. Here, the authors unlock the hidden chemical space via a high entropy strategy, enabling stable long-term battery cycling.
- Sung-Kyun Jung
- , Hyeokjo Gwon
- & Ju-Sik Kim
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Article
| Open AccessCO2 electroreduction to multicarbon products in strongly acidic electrolyte via synergistically modulating the local microenvironment
Attaining high selectivity for CO2 electroreduction in acid is usually difficult due to competing hydrogen evolution. Here, the authors demonstrate efficient CO2 reduction to multicarbon products in strongly acidic medium (pH ≤ 1) on a porous Cu catalyst by combining confinement and cation effects.
- Zesong Ma
- , Zhilong Yang
- & Hongwen Huang
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Article
| Open AccessWater induced ultrathin Mo2C nanosheets with high-density grain boundaries for enhanced hydrogen evolution
Probing the direct effect of grain boundaries as active catalytic sites is very challenging. Here, the authors reveal that the dz2 orbital energy level of Mo atoms in grain boundaries exhibits an intrinsic relationship with the hydrogen evolution activity.
- Yang Yang
- , Yumin Qian
- & Xiujun Fan
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Article
| Open AccessEngineered disorder in CO2 photocatalysis
Developing an efficient photocatalyst for CO2 reduction is appealing. Here, the authors report a core-shell c-TiO2@a-TiO2-x(OH)y heterostructure with surface frustrated Lewis pairs on amorphous shells which enables a new genre of chemical reactivity.
- Zhao Li
- , Chengliang Mao
- & Geoffrey A. Ozin
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Article
| Open AccessBreaking through water-splitting bottlenecks over carbon nitride with fluorination
Graphitic carbon nitride has long been considered a poor oxygen evolution catalyst. Here, the authors report a simple fluorination strategy to prevent the accumulation of inert C=O on carbon nitride to break through this bottleneck.
- Ji Wu
- , Zhonghuan Liu
- & Yongsheng Yan
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Article
| Open AccessLithium hexamethyldisilazide as electrolyte additive for efficient cycling of high-voltage non-aqueous lithium metal batteries
High-voltage non-aqueous lithium metal batteries suffer from poor cycling stability due to the presence of impurities in the electrolyte solution. Here, the authors report lithium hexamethyldisilazide to scavenge HF and H2O, prevent the Ni dissolution and suppress side reactions during cycling.
- Danfeng Zhang
- , Ming Liu
- & Yan-Bing He