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Extrinsic hydrophobicity-controlled silver nanoparticles as efficient and stable catalysts for CO2 electrolysis
A key factor for the electrochemical reduction of CO2 to CO is limiting the competing H2 evolution reaction. Here, authors use real-time synchrotron X-ray computed tomography to show that a silver nanoparticle-ligand catalyst structure improves water management, thereby maintaining CO production.
- Young-Jin Ko
- , Chulwan Lim
- & Hyung-Suk Oh
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Hybridizing carbonate and ether at molecular scales for high-energy and high-safety lithium metal batteries
Here, authors report a linear functionalized solvent through molecular hybridization. Complementary ethers and carbonates are integrated into a single molecule, exhibiting properties suited for high-energy and high safety lithium metal batteries.
- Jiawei Chen
- , Daoming Zhang
- & Yongyao Xia
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Manipulating the diffusion energy barrier at the lithium metal electrolyte interface for dendrite-free long-life batteries
Constructing an artificial solid electrolyte interphase to protect the lithium metal electrode is promising but challenging. Here, authors report a facile approach to form a layer to simultaneously overcome diffusion and advection-limited ion transport to achieve dendrite-free Li plating/stripping.
- Jyotshna Pokharel
- , Arthur Cresce
- & Yue Zhou
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Electrochemically coupled CH4 and CO2 consumption driven by microbial processes
The microbial valorisation of greenhouse gases could offer promising approaches climate change mitigation. Here, authors demonstrate the coupling of methane oxidation and carbon dioxide reduction by microbial consortia, facilitated by the redox cycling of iron minerals.
- Yue Zheng
- , Huan Wang
- & Feng Zhao
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Surface 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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Ligand-modified nanoparticle surfaces influence CO electroreduction selectivity
Enhancing the kinetics and selectivity of CO2/CO electroreduction towards valuable multi-carbon products poses a scientific challenge and is imperative for practical applicability. Here the authors report that modifying copper catalysts with surface thiol ligands significantly improves acetate selectivity.
- Erfan Shirzadi
- , Qiu Jin
- & Edward H. Sargent
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Efficient bubble/precipitate traffic enables stable seawater reduction electrocatalysis at industrial-level current densities
Seawater electroreduction is a promising technique for producing hydrogen, but it is hindered by cathodic Mg2 + /Ca2+ precipitation. Here, the authors propose a microscopic bubble/precipitate traffic system that releases small-sized bubbles across the cathode to repel Mg2 + /Ca2+ precipitates from almost the entire surface area of the catalyst.
- Jie Liang
- , Zhengwei Cai
- & Bo Tang
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Activating reversible carbonate reactions in Nasicon solid electrolyte-based Na-air battery via in-situ formed catholyte
Metal-air batteries, operated in ambient air, suffer from irreversible redox reactions, limiting their energy density. Herein, the authors present a solid electrolyte-based sodium-air battery with a reversible carbonate reaction, facilitated by the in-situ formed catholyte enabled by moisture.
- Heetaek Park
- , Minseok Kang
- & Byoungwoo Kang
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Aluminum 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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Paired electrocatalysis unlocks cross-dehydrogenative coupling of C(sp3)-H bonds using a pentacoordinated cobalt-salen catalyst
Cross-dehydrogenative coupling (CDC) of C-H bonds is an ideal approach for C-C bond construction but suffers from low selectivity of similar C-H bonds. Here, the authors describe a highly selective paired electrocatalysis strategy towards CDC combining hydrogen evolution reaction catalysis with hydride transfer catalysis.
- Ke Liu
- , Mengna Lei
- & Sheng Zhang
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Pd/NiMoO4/NF electrocatalysts for the efficient and ultra-stable synthesis and electrolyte-assisted extraction of glycolate
Here, the authors report a path for electrocatalytic conversions of alcohols through in-situ acid-base reaction and the design of electrocatalysts. In this work, the electrocatalyst had reduced Pd content, improved efficiency, and lowered costs.
- Kai Shi
- , Di Si
- & Jianlin Shi
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The formation of unsaturated IrOx in SrIrO3 by cobalt-doping for acidic oxygen evolution reaction
SrIrO3-based catalyst is a promising candidate for acidic oxygen evolution reaction (OER), but the active sites and factors responsible for its effectiveness remain ambiguous. Here, the authors reveal that dynamic dissolution of Co in Co-SrIrO3 leads to the formation of unsaturated IrOx, enabling high-efficiency OER.
- Jia-Wei Zhao
- , Kaihang Yue
- & Gao-Ren Li
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Enhancement 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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Electroreduction of unactivated alkenes using water as hydrogen source
The reduction of unactivated alkyl alkenes is a difficult challenge in organic chemistry. Here, the authors present a silicon-mediated electroreduction of alkyl alkenes, using water as a hydrogen source, enabled by [Fe]-H.
- Yanwei Wang
- , Qian Wang
- & Youai Qiu
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Dynamical evolution of CO2 and H2O on garnet electrolyte elucidated by ambient pressure X-ray spectroscopies
Li6.5La3Zr1.5Ta0.5O12 (LLZO) is a promising solid electrolyte but suffers from severe surface degradation in air. Here, authors use mapping of resonant Auger spectroscopy and various ambient pressure X-ray spectroscopies to elucidate the dynamical evolution of CO2 and H2O on clean LLZO surfaces.
- Nian Zhang
- , Guoxi Ren
- & Xiaosong Liu
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Autonomous closed-loop mechanistic investigation of molecular electrochemistry via automation
Electrochemical research often requires stringent combinations of experimental parameters that are demanding to manually locate. Here the authors report an autonomous electrochemical platform that implements an adaptive, closed-loop workflow for mechanistic investigation of molecular electrochemistry.
- Hongyuan Sheng
- , Jingwen Sun
- & Chong Liu
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Single [0001]-oriented zinc metal anode enables sustainable zinc batteries
The authors present a single [0001]-oriented Zn metal anode with high reversibility and demonstrate the significance of the Zn(0002) metal anode, characterized by a single crystalline orientation, for promoting ultra-sustainable homoepitaxial growth.
- Xiaotan Zhang
- , Jiangxu Li
- & Jiang Zhou
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Efficient palladium-catalyzed electrocarboxylation enables late-stage carbon isotope labelling
Carbon isotope labelling of bioactive molecules is essential for accessing the pharmacokinetic and pharmacodynamic properties of new drug entities. Here, the authors propose an electrochemical isotope-labelling protocol which enables the use of near-stoichiometric 14CO2, facilitating late-stage and single-step carbon-14 labelling of pharmaceuticals and representative precursors.
- Gabriel M. F. Batista
- , Ruth Ebenbauer
- & Troels Skrydstrup
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Deciphering 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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Single-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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An entanglement association polymer electrolyte for Li-metal batteries
Here, the authors report an entanglement association polymer electrolyte with a polymer matrix and copolymer stabilizer. The developed entangled structure forms a stable interface for the polymer electrolyte during charging and discharging.
- Hangchao Wang
- , Yali Yang
- & Dingguo Xia
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Locking the lattice oxygen in RuO2 to stabilize highly active Ru sites in acidic water oxidation
RuO2 is highly active toward the acidic electrochemical oxygen evolution reaction but exhibits instability due to lattice oxygen oxidation. Here, authors prepare an interstitial Si-decorated RuO2 catalyst with improved stability for acidic water oxidation by suppressing lattice oxygen oxidation.
- Xinyu Ping
- , Yongduo Liu
- & Zidong Wei
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Pulse potential mediated selectivity for the electrocatalytic oxidation of glycerol to glyceric acid
Mitigating the deactivation of noble metal-based catalysts caused by self-oxidation and toxic adsorption poses a considerable challenge in organic electro-oxidation. This study addresses the issue by employing a pulsed potential electrolysis approach to selectively electrocatalyze the oxidation of glycerol to glyceric acid using a Pt-based catalyst.
- Wei Chen
- , Liang Zhang
- & Yuqin Zou
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Phenol as proton shuttle and buffer for lithium-mediated ammonia electrosynthesis
The proton shuttle plays a critical role in the proton transfer process during lithium-mediated ammonia synthesis. Here, the authors establish the structure-activity relationship and design principles for effective proton shuttles.
- Xianbiao Fu
- , Aoni Xu
- & Ib Chorkendorff
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A solid-state lithium-ion battery with micron-sized silicon anode operating free from external pressure
Applying high stack pressure is primarily done to address the mechanical failure issue of solid-state batteries. Here, the authors propose a mechanical optimization strategy involving elastic electrolyte to realize solid-state batteries operating without external pressurizing.
- Hui Pan
- , Lei Wang
- & Haoshen Zhou
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Inter-site structural heterogeneity induction of single atom Fe catalysts for robust oxygen reduction
Here, authors report an inter-site structural heterogeneity induced effect of hierarchical single atom Fe catalysts for robust oxygen reduction. Dynamic evolutions and insights into structure-activity relationship are presented.
- Peng Zhang
- , Hsiao-Chien Chen
- & Yuan Pan
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Molecular anchoring of free solvents for high-voltage and high-safety lithium metal batteries
Advanced electrolyte is essential for high-energy-density lithium metal batteries. Here, the authors design a molecular anchoring dilute electrolyte via intermolecular hydrogen bonding with free solvents to improve the battery electrochemical and thermal stabilities.
- Zhuangzhuang Cui
- , Zhuangzhuang Jia
- & Xiaodi Ren
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Dynamic chloride ion adsorption on single iridium atom boosts seawater oxidation catalysis
The seawater oxidation reaction faces challenges from competitive chloride oxidation reaction. Herein, the authors have utilized chlorine adsorption to modulate the single-atom Ir coordination state and promote seawater oxidation and catalyst stability.
- Xinxuan Duan
- , Qihao Sha
- & Xiaoming Sun
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Cation desolvation-induced capacitance enhancement in reduced graphene oxide (rGO)
Understanding local electrochemical processes can help improve electrochemical energy storage. Here, the authors report a charge storage mechanism in aqueous electrolyte for reduced graphene oxide using an electrochemical quartz crystal microbalance.
- Kangkang Ge
- , Hui Shao
- & Patrice Simon
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Influence of electric double layer rigidity on CO adsorption and electroreduction rate
High-pressure infrared spectroscopy shows concentrated cations suppress CO adsorption. Here the authors report two electrochemical interfaces forming distinct double layer structures and reaction rates at elevating pressure and various potentials.
- Jiajie Hou
- , Bingjun Xu
- & Qi Lu
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Single-atom tailored atomically-precise nanoclusters for enhanced electrochemical reduction of CO2-to-CO activity
Tailoring catalytic performance of atomically-precise metal nanoclusters catalysts is of great interest but remains challenging. Here, the authors report a co-eletropolymerization strategy to modify well-defined Au8 nanoclusters by single-atom sites to enhance its electrocatalytic activity for the reduction of CO2 towards CO.
- Yi-Man Wang
- , Fang-Qin Yan
- & Shuang-Quan Zang
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Continuous strain tuning of oxygen evolution catalysts with anisotropic thermal expansion
Tuning compressive strain is an effective way to accelerate the oxygen evolution reaction kinetics. Here the authors show that anisotropic thermal expansion induces compressive strains on IrO6 octahedron in Sr2IrO4, shifting its d-band center downward and accelerating water oxidation kinetics beyond traditional thermal diffusion effects.
- Yu Du
- , Fakang Xie
- & Zhigang Zou
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In situ copper faceting enables efficient CO2/CO electrolysis
Copper electrocatalysts enable carbon dioxide/carbon monoxide reduction but suffer from low production rates. Here, the authors promote in situ growth of Cu(100) during electrolysis, enabling efficient and stable electrosynthesis of multicarbon products at industrially-relevant current densities
- Kaili Yao
- , Jun Li
- & Hongyan Liang
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Nanocurvature-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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Creation of a point-of-care therapeutics sensor using protein engineering, electrochemical sensing and electronic integration
Low-cost point-of-care sensors are vital for precision medicine. Here, the authors have repurposed a glucometer for breast cancer therapeutic detection capable of sensing tamoxifen in human blood, utilizing blood glucose to power and amplify the therapeutic signals
- Rong Cai
- , Chiagoziem Ngwadom
- & Caroline M. Ajo-Franklin
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Efficient direct repairing of lithium- and manganese-rich cathodes by concentrated solar radiation
Rapid capacity decay and voltage drop hinder lithium- and manganese-rich cathode material (LMRO) development. Here, the authors apply concentrated solar radiation arrays on cycled LMRO electrodes, inducing inverse spinel phase to boost redox activity and reversibility, yielding enhanced electrochemical performance.
- Hailong Wang
- , Xin Geng
- & Xin He
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Unveiling the nature of Pt-induced anti-deactivation of Ru for alkaline hydrogen oxidation reaction
Despite the high intrinsic activity of Ru for hydrogen oxidation reaction, the surface oxidation-induced deactivation limits the application. Here, the authors report the introduction of Pt atoms could prevent the surface oxidation-related interfacial water network damage, preventing the deactivation of Ru.
- Yanyan Fang
- , Cong Wei
- & Gongming Wang
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Liquid Madelung energy accounts for the huge potential shift in electrochemical systems
Electrode potential in any electrochemical systems has long been discussed by classical Debye-Hückel theory which holds only under extremely dilute concentrations. Here, the authors establish the concept ‘liquid Madelung potential’ to comprehensively describe the potential shift at practical concentrations.
- Norio Takenaka
- , Seongjae Ko
- & Atsuo Yamada
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Promoting high-voltage stability through local lattice distortion of halide solid electrolytes
Solid electrolytes play a crucial role as ion conductors and separator between electrodes in all-solid-state batteries. Here, the authors report a high-entropy halide solid electrolyte, which reveals the structure evolution with the increasing configurational entropy and improves the high-voltage stability.
- Zhenyou Song
- , Tengrui Wang
- & Wei Luo
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Oxygen-tolerant CO2 electroreduction over covalent organic frameworks via photoswitching control oxygen passivation strategy
Direct use of flue gas for the electrocatalytic CO2 reduction reaction is desirable but severely limited by the thermodynamically favorable oxygen reduction reaction. Here the authors report an oxygen passivation strategy to improve electrocatalytic CO2 reduction reaction under aerobic conditions using a covalent organic frameworks with a photoswitching unit.
- Hong-Jing Zhu
- , Duan-Hui Si
- & Yuan-Biao Huang
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Facilitating alkaline hydrogen evolution reaction on the hetero-interfaced Ru/RuO2 through Pt single atoms doping
Exploring an active and cost-effective catalyst for alkaline hydrogen evolution reaction remains elusive to date. Here, the authors report the platinum single-atoms doped ruthenium/ruthenium oxides showing distinctly enhanced catalytic performance.
- Yiming Zhu
- , Malte Klingenhof
- & Jiwei Ma
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High-spin Co3+ in cobalt oxyhydroxide for efficient water oxidation
Regulating spin state of metal cations in catalysts is recognized as a strategy to improve water oxidation. Herein, the authors constructed high-spin cobalt ions in cobalt oxyhydroxides, experimentally demonstrating accelerated electron transfer ability and thereby superior water oxidation performance.
- Xin Zhang
- , Haoyin Zhong
- & Junmin Xue
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Electrocatalytic water oxidation with manganese phosphates
Understanding water oxidation on Mn-based catalysts remains a long-standing challenge. Here, the authors use homologous KMnPO4 and KMnPO4•H2O as model catalyst to show that Mn(V)=O is responsible for O−O bond formation and its concentration determines the intrinsic activity.
- Shujiao Yang
- , Kaihang Yue
- & Wei Zhang
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Ca-dimers, solvent layering, and dominant electrochemically active species in Ca(BH4)2 in THF
Alternatives to lithium-ion electrochemistry present challenges due to undesirable phenomena at the electrode-electrolyte interface. Through simulations, the authors find that the performance of a calcium-based electrolyte is driven entirely by molecular-scale processes within approximately 1 nm of the electrode.
- Ana Sanz Matias
- , Fabrice Roncoroni
- & David Prendergast
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Hierarchical Li electrochemistry using alloy-type anode for high-energy-density Li metal batteries
Utilizing an ultra-thin Li anode with a thickness below 50 μm is crucial for enhancing the energy density of batteries. Here, the authors develop a finely tunable, thin alloy-based Li anode that features a hierarchical Li electrochemistry, enabling stable cycling and superior energy density in Li metal batteries.
- Jiaqi Cao
- , Yuansheng Shi
- & Xia Lu
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Solvation-property relationship of lithium-sulphur battery electrolytes
In the Li-S battery, a promising next-generation battery chemistry, electrolytes are vital because of solvated polysulfide species. Here, the authors investigate solvation-property relationships via the measurement of solvation free energy of the electrolytes, guiding advanced electrolyte design for Li-S batteries.
- Sang Cheol Kim
- , Xin Gao
- & Yi Cui
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A surface strategy boosting the ethylene selectivity for CO2 reduction and in situ mechanistic insights
The electrochemical reduction of CO2 into multi-carbon product is interesting yet requires further research. Here, the authors develop a surface strategy to achieve high CO2-to-ethylene selectivity by dodecanethiol modification CuO electrode and show that dodecanethiol facilitates CO2 transfer, enhances *CO coverage and stabilize Cu(100) facet.
- Yinchao Yao
- , Tong Shi
- & Zhuo Chen
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Acidic 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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Redox-tunable isoindigos for electrochemically mediated carbon capture
Electrochemically-mediated carbon capture has good energy efficiency and potential in carbon dioxide separation, but optimisation of these systems is challenging. Here, the authors report the use of isoindigo derivatives to give fine-tuned interactions with CO2 for carbon capture methods.
- Xing Li
- , Xunhua Zhao
- & Yayuan Liu
Electric-field-assisted proton coupling enhanced oxygen evolution reaction