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| Open AccessImproving rechargeable magnesium batteries through dual cation co-intercalation strategy
Rechargeable magnesium batteries suffer from poor mobility of Mg-ions, severely affecting the electrochemical performance. Here, authors demonstrate a strategy of co-intercalation of monovalent ions into the host lattice, which substantially improves Mg-ion mobility and battery performance.
- Ananyo Roy
- , Mohsen Sotoudeh
- & Zhenyou Li
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Article
| Open AccessSynergistic dual-phase air electrode enables high and durable performance of reversible proton ceramic electrochemical cells
Efficient air electrodes drive reversible proton ceramic electrochemical cells, accelerating renewable energy conversion and storage. Here, the authors propose a highly active hybrid air electrode that effectively controls phase content, enhancing electrochemical activity and stability through synergistic effects.
- Zuoqing Liu
- , Yuesheng Bai
- & Zongping Shao
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Article
| Open AccessCobalt-free composite-structured cathodes with lithium-stoichiometry control for sustainable lithium-ion batteries
As electric vehicle batteries adopt cobalt-free layered cathodes to tackle supply chain issues, it greatly impacts battery lifespan. Here, the authors develop a lithium stoichiometry control method to synthesize cobalt-free composite-structured cathodes with high cycling stability, enabling long-life sustainable batteries.
- Ke Chen
- , Pallab Barai
- & Feng Wang
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Article
| Open AccessA replacement strategy for regulating local environment of single-atom Co-SxN4−x catalysts to facilitate CO2 electroreduction
The local coordination environment determines the properties of single-atom catalysts. Here, authors develop a thermal replacement method to fine tune the coordination structure of cobalt-based single-atom catalysts and study their activity toward carbon dioxide electroreduction.
- Jiajing Pei
- , Huishan Shang
- & Zhongbin Zhuang
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Article
| Open AccessMachine-learning-accelerated design of high-performance platinum intermetallic nanoparticle fuel cell catalysts
Platinum-based intermetallic alloys are promising candidates as low-platinum oxygen reduction reaction catalysts for proton exchange membrane fuel cells. Here, the authors develop small sized and highly ordered Pt2CoCu and Pt2CoNi catalysts for fuel cells by machine-learning accelerated computational screening.
- Peng Yin
- , Xiangfu Niu
- & Hai-Wei Liang
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Article
| Open AccessInterfacial self-healing polymer electrolytes for long-cycle solid-state lithium-sulfur batteries
Low ion conductivity, large interfacial resistance, and dendrite growth hinder the practical use of solid-state batteries. Here, the authors introduce a self-healing poly(ether-urethane)-based solid-state polymer electrolyte to address these issues, resulting in high performance solid-state lithium-sulfur batteries.
- Fei Pei
- , Lin Wu
- & Yunhui Huang
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Article
| Open AccessA weakly solvating electrolyte towards practical rechargeable aqueous zinc-ion batteries
The practical deployment of aqueous zinc-ion batteries is hindered by the structure deterioration and side reactions at electrodes. Here, the authors introduce a weakly solvating electrolyte with butanone as an electrolyte additive to stabilize both the cathode and anode of aqueous zinc-ion batteries simultaneously.
- Xin Shi
- , Jinhao Xie
- & Xihong Lu
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Article
| Open AccessOperando formation of highly efficient electrocatalysts induced by heteroatom leaching
Stability of catalyst dopant species under working conditions is often unexplored. Here, the authors reveal that the dopant sites tend to collapse when the applied potential is too negative or too positive and describe a protocol for the in-situ formation of highly efficient active sites via the leaching of dopants.
- Cong Liu
- , Bingbao Mei
- & Weilin Xu
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Article
| Open AccessSpin-related Cu-Co pair to increase electrochemical ammonia generation on high-entropy oxides
Electrochemical conversion of nitrate into ammonia offers a method for mitigating nitrate pollution in water. Here the authors report the electrochemical nitrate-to-ammonia conversion using high-entropy oxide Mg0.2Co0.2Ni0.2Cu0.2Zn0.2O and find that the Co spin states are crucial for synergistic ammonia generation.
- Shengnan Sun
- , Chencheng Dai
- & Zhi Wei Seh
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Article
| Open AccessVitamin C-induced CO2 capture enables high-rate ethylene production in CO2 electroreduction
Efficiently producing multicarbon chemicals through electrochemical CO2 reduction is essential for achieving economically feasible carbon neutrality. Here, the authors present molecularly enhanced CO2-to-*CO conversion and *CO dimerization for high-rate ethylene production by nanoconfinement of ascorbic acid.
- Jongyoun Kim
- , Taemin Lee
- & Dae-Hyun Nam
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Article
| Open AccessSequential co-reduction of nitrate and carbon dioxide enables selective urea electrosynthesis
Electrochemical co-reduction of nitrate and carbon dioxide is a promising approach for urea synthesis. Here, the authors report a sequential co-reduction strategy for catalyst design that can dynamically adjust the competition between the two reduction processes, resulting in a high selectivity towards urea.
- Yang Li
- , Shisheng Zheng
- & Shunning Li
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Article
| Open AccessSpin polarized Fe1−Ti pairs for highly efficient electroreduction nitrate to ammonia
Electrochemical nitrate reduction to ammonia offers an attractive solution to environmental sustainability and clean energy production. Here, the authors construct spin−polarized Fe1−Ti pairs via manipulating oxygen vacancies on monolithic titanium electrode for highly efficient nitrate to ammonia conversion.
- Jie Dai
- , Yawen Tong
- & Lizhi Zhang
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Article
| Open AccessMetal-support interaction boosts the stability of Ni-based electrocatalysts for alkaline hydrogen oxidation
Nickel-based electrocatalysts for hydrogen oxidation in anion exchange membrane fuel cells face stability issues. Here the authors report Ni4Mo/TiO2 catalyst with significantly improved stability, owing to the efficient charge transfer from TiO2 to Ni.
- Xiaoyu Tian
- , Renjie Ren
- & Wenchao Sheng
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Article
| Open AccessAsynchronous domain dynamics and equilibration in layered oxide battery cathode
The battery performance at the cell level is an integration of contributions from many active particles. Here, the authors present a direct visualization of the active cathode particles that react heterogeneously and asynchronously by using coherent multi-crystal diffraction and optical microscopy.
- Zhichen Xue
- , Nikhil Sharma
- & Yijin Liu
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Article
| Open AccessCapturing critical gem-diol intermediates and hydride transfer for anodic hydrogen production from 5-hydroxymethylfurfural
The detailed mechanism of anodic H2 production from aldehydes remains unclear. Here, authors identify two key interconvertible intermediates of 5-hydroxymethylfurfural oxidation in alkaline medium, finding H2 production via hydride transfer from one of the intermediates.
- Guodong Fu
- , Xiaomin Kang
- & Jing-Li Luo
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Article
| Open AccessAn inorganic-rich but LiF-free interphase for fast charging and long cycle life lithium metal batteries
Fluorinated interphases are often pursued as a design strategy for Li metal batteries. In contrast, here the authors show that an electrolyte with a non-fluorinated solvent and CsNO3 additive results in an LiF-free but inorganic-rich interphase that enables fast-charging of Li metal batteries.
- Muhammad Mominur Rahman
- , Sha Tan
- & Enyuan Hu
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Article
| Open AccessDiscovery of fast and stable proton storage in bulk hexagonal molybdenum oxide
Nanostructured electrode materials pose several challenges, including poor volumetric performance, severe side reactions, high costs, and complexity. Here, the authors develop a micrometer-sized bulk hexagonal molybdenum oxide with unconventional charge storage mechanism for fast and stable proton storage.
- Tiezhu Xu
- , Zhenming Xu
- & Laifa Shen
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Article
| Open AccessBreaking solvation dominance of ethylene carbonate via molecular charge engineering enables lower temperature battery
Low-temperature operation remains challenging for batteries. Here, the authors report an electrolyte solvation structure design strategy to break solvation dominance of ethylene carbonate to facilitate the desolvation process that improves the low-temperature performance of lithium-ion batteries even below −100 °C.
- Yuqing Chen
- , Qiu He
- & Jilei Liu
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Article
| Open AccessElectroreductive hydroxy fluorosulfonylation of alkenes
As sulfonyl fluorides have found wide applications, synthetic access to β-hydroxy sulfonyl fluorides is desirable. Here, the authors report an electroreductive strategy for radical hydroxyl fluorosulfonylation of alkenes with sulfuryl chlorofluoride and molecular oxygen from air.
- Qingyuan Feng
- , Tianyu He
- & Shenlin Huang
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Article
| Open AccessCrystal-facet-dependent surface transformation dictates the oxygen evolution reaction activity in lanthanum nickelate
The development of active and stable catalysts for water splitting requires understanding of the surface transformations that occur during the reaction. Here, the authors report how the transformations and the activity depend on the exposed crystal facet using spectroscopy and ab initio calculations.
- Achim Füngerlings
- , Marcus Wohlgemuth
- & Christoph Baeumer
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Article
| Open AccessA corrosion inhibiting layer to tackle the irreversible lithium loss in lithium metal batteries
Lithium metal electrodes suffer from both chemical and electrochemical corrosion during battery storage and operation. Here, the authors show that lithium corrosion is due to dissolution of the solid-electrolyte interphase and suppress this by utilizing a multifunctional passivation layer.
- Chengbin Jin
- , Yiyu Huang
- & Xinyong Tao
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Article
| Open AccessStabilizing ruthenium dioxide with cation-anchored sulfate for durable oxygen evolution in proton-exchange membrane water electrolyzers
Designing stable Ru-based catalysts for acidic oxygen evolution remains a challenge. Here, the authors propose an oxyanion protection strategy to prevent the formation of oxygen vacancies on the RuO2 surface by creating coordination-saturated lattice oxygen, thereby greatly enhancing the stability.
- Yanrong Xue
- , Jiwu Zhao
- & Xu Lu
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Article
| Open AccessDefective oxygen inert phase stabilized high-voltage nickel-rich cathode for high-energy lithium-ion batteries
The oxygen evolutions from layered cathode surfaces cause battery degradation during high-voltage operation and pose thermal safety concerns. Here, the authors propose a strategy to anchor and reserve surface oxygen with defective oxygen inert phase for high-voltage nickel-rich cathodes in lithium-ion batteries.
- Zhongsheng Dai
- , Zhujie Li
- & Li Li
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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 AccessSelective C(sp3)–H arylation/alkylation of alkanes enabled by paired electrocatalysis
The combination of electrochemistry and photochemistry in the context of organic synthesis is in its infancy. Here, the authors report selective C(sp3)–H arylation/alkylation of alkanes, using Earth-abundant bimetallic transition metal catalysis, under photo- and electrochemical conditions.
- Long Zou
- , Siqi Xiang
- & Qingquan Lu
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Article
| Open AccessUnraveling the synergistic effects of Cu-Ag tandem catalysts during electrochemical CO2 reduction using nanofocused X-ray probes
Combining in situ nanoprobe techniques paves the way for gaining insights into structure-selectivity relations for electrocatalysts. Herein, the dynamic evolution of lattice strain in individual nanoparticles is directly visualized with nanoscale resolution in Cu-Ag tandem catalysts during the electrocatalytic conversion of CO2 into value-added chemicals.
- Marvin L. Frisch
- , Longfei Wu
- & Peter Strasser
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Article
| Open AccessAtomic-level polarization in electric fields of defects for electrocatalysis
The visible evidence bridging atomic defects with catalytic properties has been scarcely explored. Using differential phase contrast technology, this work discloses the existence of a polarized electric field surrounding the antisite defects of a monolayer MoS2 material and its correlation to its electrocatalytic hydrogen evolution property.
- Jie Xu
- , Xiong-Xiong Xue
- & Jun Lu
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Article
| Open AccessCooperative Fe sites on transition metal (oxy)hydroxides drive high oxygen evolution activity in base
Fe-based oxyhydroxides are promising catalysts for oxygen evolution reactions. However, the dynamics of Fe sites require further investigation. Here, the authors report Fe oxyhydroxide clusters on nickel or cobalt oxyhydroxides as key active sites for water oxidation and reveal how these clusters are selectively formed under controlled electrochemical conditions.
- Yingqing Ou
- , Liam P. Twight
- & Shannon W. Boettcher
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| Open AccessDirect OC-CHO coupling towards highly C2+ products selective electroreduction over stable Cu0/Cu2+ interface
The electrosynthesis of multicarbon products from CO2 is a highly attractive way to utilize emitted CO2. Here, the authors report in situ formed Cu0/Cu2+ interfaces from copper phosphate-based electrocatalysts for promoting selectivity toward multicarbon products through OC-CHO coupling.
- Xin Yu Zhang
- , Zhen Xin Lou
- & Hua Gui Yang
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Article
| Open AccessStabilizing non-iridium active sites by non-stoichiometric oxide for acidic water oxidation at high current density
Developing stable and efficient non-iridium-based acidic oxygen evolution reaction electrocatalysts is crucial but challenging. Here, we report that non-stoichiometric Ti oxides can safeguard the Ru sites through charge-redistribution, thereby enhancing the catalytic performance.
- Lingxi Zhou
- , Yangfan Shao
- & Ruitao Lv
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Article
| Open AccessAtomic-scale probing of short-range order and its impact on electrochemical properties in cation-disordered oxide cathodes
Derivation of atomic arrangements of short-range-order from diffused intensity pattern in reciprocal space for Li-excess cation-disordered rocksalt cathode remains as a challenge. Here, the authors reveal the short-range-order is a convolution of three basic types: tetrahedron, octahedron, and cube.
- Linze Li
- , Bin Ouyang
- & Chongmin Wang
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Article
| Open AccessEnhanced copper anticorrosion from Janus-doped bilayer graphene
Atomically thick anticorrosion coatings on Cu are desired for future applications, but still at its infancy. Here, the authors report a Janus-doping mechanism in bilayer graphene on Cu substrate that results in an enhanced anticorrosion performance.
- Mengze Zhao
- , Zhibin Zhang
- & Kaihui Liu
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Article
| Open AccessAccelerating multielectron reduction at CuxO nanograins interfaces with controlled local electric field
Controlling the kinetics and thermodynamics of electrochemical processes is essential to achieve high-performance multielectron reduction. Here, the authors report laser-induced copper bipyramids with abundant nanograins and controlled tip angles for enhanced multielectron CO2 and nitrate reduction.
- Weihua Guo
- , Siwei Zhang
- & Ruquan Ye
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Article
| Open AccessPulsed electroreduction of low-concentration nitrate to ammonia
Electrocatalytic nitrate reduction to ammonia has emerged as an alternative strategy for effluent treatment and ammonia production. Here, the authors report a pulsed potential approach to overcome the sluggish reaction kinetics caused by the limited distribution of negatively charged nitrate near the working electrode and the competing side reactions.
- Yanmei Huang
- , Caihong He
- & Yifu Yu
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Article
| Open AccessDetangling electrolyte chemical dynamics in lithium sulfur batteries by operando monitoring with optical resonance combs
The shuttle effect of polysulfides in lithium sulfur batteries leads to performance degradation. Here, authors use fiber-based sensors to track and quantify the dissolved polysulfide concentration in the electrolyte during cell charge and discharge, revealing insights on stability and performance.
- Fu Liu
- , Wenqing Lu
- & Jean-Marie Tarascon
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Article
| Open AccessOperando Li metal plating diagnostics via MHz band electromagnetics
Internal growth of Li-metal deposition is critical for evaluating the state of safety in lithium-ion batteries. Here the authors show a Li-metal detection method utilizing high-frequency electromagnetics, which can be assembled as a sensor for monitoring cycle-by-cycle growth of Li-metal plating.
- Masanori Ishigaki
- , Keisuke Ishikawa
- & Tsuyoshi Sasaki
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Article
| Open AccessElectrocatalytic valorization of lignocellulose-derived aromatics at industrial-scale current densities
The authors report a flow-cell system equipped with highly-electrolyte permeable Rh diffusion cathode for electrocatalytic hydrogenation of important bio-oil aromatic molecules at industrial-scale current densities.
- Tao Peng
- , Wenbin Zhang
- & Wei Zhao
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Article
| Open AccessTailoring chemical composition of solid electrolyte interphase by selective dissolution for long-life micron-sized silicon anode
The severe volume expansion during the lithiation of micron-sized Si in Li-ion batteries requires a solid electrolyte interphase with reinforced mechanical stability. Here, the authors propose a solvent-induced selective dissolution strategy to regulate the mechanical properties of the interphase.
- Yi-Fan Tian
- , Shuang-Jie Tan
- & Yu-Guo Guo
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Article
| Open AccessTailoring grain boundary stability of zinc-titanium alloy for long-lasting aqueous zinc batteries
The electrochemical performance of metal electrodes is significantly influenced by their grain boundary stability. Here, the authors propose a zinc-titanium two-phase alloy via grain boundary engineering to inhibit intergranular corrosion and tailor deposition behavior for stable aqueous zinc batteries.
- Yunxiang Zhao
- , Shan Guo
- & Jiang Zhou
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Article
| Open AccessAccelerated deprotonation with a hydroxy-silicon alkali solid for rechargeable zinc-air batteries
Surface reconstruction caused by adsorbate evolution mechanism leads to poor oxygen evolution reaction (OER) performance. Here, the authors introduce a hydroxy-silicon proton acceptor as OER catalyst which greatly accelerates the deprotonation process in OER and prolong the cycle life of zinc-ion batteries.
- Yaobin Wang
- , Xinlei Ge
- & Yunfei Bu
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Article
| Open AccessDefects and nanostrain gradients control phase transition mechanisms in single crystal high-voltage lithium spinel
Lithiation dynamics and phase transition mechanisms in battery materials remain poorly understood. Here authors use operando X-ray nanodiffraction microscopy to reveal how domains relate to defects and how cycling affects the lattice domain reorientation in LiMn1.5Ni0.5O4 single crystals.
- Isaac Martens
- , Nikita Vostrov
- & Tobias U. Schulli
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Article
| Open AccessOrganomediated electrochemical fluorosulfonylation of aryl triflates via selective C–O bond cleavage
Although aryl triflates are essential building blocks in organic synthesis, the applications as aryl radical precursors are limited. Here, the authors report an organomediated electrochemical strategy for the generation of aryl radicals from aryl triflates, providing a method for the synthesis of aryl sulfonyl fluorides from feedstock phenol derivatives under very mild conditions.
- Xianqiang Kong
- , Yiyi Chen
- & Zhong-Yan Cao
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Article
| Open AccessRevealing the role of double-layer microenvironments in pH-dependent oxygen reduction activity over metal-nitrogen-carbon catalysts
By combining theoretical simulations and spectroscopic measurements, Peng Li et al. demonstrated that distinct interfacial double-layer structures play a key role in the pH-dependent oxygen reduction kinetics over metal-nitrogen-carbon catalysts.
- Peng Li
- , Yuzhou Jiao
- & Shengli Chen
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Article
| Open AccessSEI growth on Lithium metal anodes in solid-state batteries quantified with coulometric titration time analysis
In lithium-metal batteries, it is vital to quantify electrolyte side reactions occurring at the metal anode surface. Here, the authors introduce an electrochemical technique, using a series of small-step lithium deposition followed by open circuit voltage analysis, to accurately measure these reactions.
- Burak Aktekin
- , Luise M. Riegger
- & Jürgen Janek
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Article
| Open AccessThe practice of reaction window in an electrocatalytic on-chip microcell
Here, the authors investigate frequently observed variations in data between different electrochemical cells using in-situ electronic/electrochemical measurements, developing a vertical microcell strategy to eliminate the conductance issue and enhance measurement reproducibility.
- Hang Xia
- , Xiaoru Sang
- & Yongmin He
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Article
| Open AccessKnowledge-driven design of solid-electrolyte interphases on lithium metal via multiscale modelling
The application of Li metal electrodes in rechargeable batteries is limited by inherent high reactivity. Here, the authors provide model-based insights into the composition and formation mechanisms of the solid-electrolyte interphase on the µs-scale and suggest design strategies for the interphase.
- Janika Wagner-Henke
- , Dacheng Kuai
- & Ulrike Krewer
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Article
| Open AccessBoosting lithium ion conductivity of antiperovskite solid electrolyte by potassium ions substitution for cation clusters
All-solid-state electrolytes for lithium batteries generally suffer from low ionic conductivity. Here, authors manipulate the lattice of antiperovskite-type Li2OHCl by potassium ion substitution, which alters the lattice structure and improves the lithium ion transport properties.
- Lei Gao
- , Xinyu Zhang
- & Ruqiang Zou
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Article
| Open AccessProlonged hydrogen production by engineered green algae photovoltaic power stations
Cost, scalability, and durability are critical factors determining the application of artificial photosynthesis systems. Here, the authors address these problems by inserting a carbon nanofiber into the chloroplast of green algae to transfer of electrons for photosynthesis and demonstrate H2 production up to 50 days.
- Hyo Jin Gwon
- , Geonwoo Park
- & Hyun S. Ahn
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Article
| Open AccessCu-catalyzed asymmetric regiodivergent electrosynthesis and its application in the enantioselective total synthesis of (-)-fumimycin
Quaternary amino acids are important building blocks and precursors of medicinal compounds. Here, the authors describe a copper-catalyzed regiodivergent electrochemical core structure-oriented crossdehydrogenative coupling reaction of Schiff bases and commercially available hydroquinones to obtain three classes of chiral quaternary amino acid derivatives
- Tian Xie
- , Jianming Huang
- & Chang Guo