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Optimizing high-coordination shell of Co-based single-atom catalysts for efficient ORR and zinc-air batteries

Journal of Energy Chemistry 2024年第8期95卷 306-314页

作者： Yugang Qi Qing Liang Kexin Song Xinyan Zhou Meiqi Liu Wenwen Li Fuxi Liu Zhou Jiang Xu Zou Zhongjun Chen Wei Zhang Weitao Zheng Key laboratory of Automobile materials MOE School of Materials Science & Engineering Electron Microscopy Center and International Center of Future Science Jilin Provincial International Cooperation Key Laboratory of High-Efficiency Clean Energy Materials Jilin University Institute of High Energy Physics Chinese Academy of Sciences

Atom-level modulation of the coordination environment for single-atom catalysts(SACs) is considered as an effective strategy for elevating the catalytic performance. For the MNxsite, breaking the symmetrical geometry and charge distribution by introducing relatively weak electronegative atoms into the first/second shell is an efficient way, but it remains challenging for elucidating the underlying mechanism of interaction. Herein, a practical strategy was reported to rationally design single cobalt atoms coordinated with both phosphorus and nitrogen atoms in a hierarchically porous carbon derived from metal-organic frameworks. X-ray absorption spectrum reveals that atomically dispersed Co sites are coordinated with four N atoms in the first shell and varying numbers of P atoms in the second shell(denoted as Co-N/P-C).The prepared catalyst exhibits excellent oxygen reduction reaction(ORR) activity as well as zinc-air battery performance. The introduction of P atoms in the Co-SACs weakens the interaction between Co and N,significantly promoting the adsorption process of *OOH, resulting in the acceleration of reaction kinetics and reduction of thermodynamic barrier, responsible for the increased intrinsic activity. Our discovery provides insights into an ultimate design of single-atom catalysts with adjustable electrocatalytic activities for efficient electrochemical energy conversion.

关键词： Electrocatalytic Oxygen reduction reaction Shell coordination optimization Single atom catalyst

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Hierarchical FeO_(χ)H_(y)@Ni_(3)B hybrid for efficient alkaline oxygen evolution at high current density

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Journal of Energy Chemistry 2024年第7期94卷 599-607页

作者： Fuxi Liu Qing Liang Zhenyu Li Meiqi Liu Naiin Yue Zizhun Wang Xu Zou Wei Zhang Key laboratory of Automobile materials Ministry of Education School of Materials Science&EngineeringElectron Microscopy CenterInternational Center of Future ScienceJilin Provincial International Cooperation Key Laboratory of High-Eficiency Clean Energy MaterialsJilin UniversityChangchun 130012JilinChina

Electrocatalysts with high activity and long-term durability are vital toward large-scale hydrogen pro-duction from electrocatalytic water splitting.Here,the self-supported electrode(FeO_(χ)H_(y)@Ni_(3)B/NF)with hierarchical heterostructure was simply prepared by using NigB chunks grown on nickel foam as sub-strate to in situ form vertical FeO_(χ)H_(y)nanosheets.Such hybrid shows efficient oxygen evolution reaction activity with overpotentials as low as 267 and 249 mV at 100 mA cm^(-2)in 1 M K0H solution and 30 wt%KOH solution,respectively.Meanwhile,it also exhibits excellent catalytic stability,sustaining catalysis at 500 mA cm^(-2)in 1 M K0H solution for 200 h,and even for 200 h at 1000 mA cm^(-2)in 30 wt%K0H solution.Further experimental results reveal that the FeO_(χ)H_(y)@Ni_(3)B/NF is endowed with superhydrophilic and superaerophobic surface properties,which not only provide more mass transport channels,as well as facilitated the diffusion of reaction intermediates and gas bubbles.Also,it holds faster reaction kinetics,more accessible active sites and accelerated electron transfer rates due to strong synergistic interactions attheheterogeneous interface.

关键词： FeO_(χ)H_(y)@Ni_(3)B/NF hybrid Heterostructure Oxygen evolution reaction Electrocatalytic

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High-efficiency sodium storage of Co_(0.85)Se/WSe_(2) encapsulated in N-doped carbon polyhedron via vacancy and heterojunction engineering

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Carbon Energy 2024年第1期6卷 94-107页

作者： Ya Ru Pei Hong Yu Zhou Ming Zhao Jian Chen Li Xin Ge Wei Zhang Chun Cheng Yang Qing Jiang Key laboratory of Automobile materials(Jilin University) Ministry of EducationSchool of Materials Science and EngineeringJilin UniversityChangchunChina Jilin Provincial international Cooperation Key laboratory of High-Efficiency Clean Energy materials Electron Microscopy CenterJilin UniversityChangchunChina

With the advantage of fast charge transfer,heterojunction engineering is identified as a viable method to reinforce the anodes'sodium storage performance.Also,vacancies can effectively strengthen the Na+adsorption ability and provide extra active sites for Na+adsorption.However,their synchronous engineering is rarely reported.Herein,a hybrid of Co_(0.85)Se/WSe_(2) heterostructure with Se vacancies and N-doped carbon polyhedron(CoWSe/NCP)has been fabricated for the first time via a hydrothermal and subsequent selenization strategy.Spherical aberration-corrected transmission electron microscopy confirms the phase interface of the Co_(0.85)Se/WSe_(2) heterostructure and the existence of Se vacancies.Density functional theory simulations reveal the accelerated charge transfer and enhanced Na+adsorption ability,which are contributed by the Co_(0.85)Se/WSe_(2) heterostructure and Se vacancies,respectively.As expected,the CoWSe/NCP anode in sodium-ion battery achieves outstanding rate capability(339.6 mAh g^(−1) at 20 A g^(−1)),outperforming almost all Co/W-based selenides.

关键词： Co_(0.85)Se/WSe_(2)heterostructure density functional theory simulations N-doped carbon polyhedron Se vacancies sodium-ion batteries

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Kinetically and thermodynamically expediting elementary steps via high-valence Cr-incorporated of nickel selenide for water electrolysis

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Nano Research 2024年第3期17卷 1199-1208页

作者： Huafeng Fan Dongxu Jiao Jinchang Fan Dewen Wang Bilal Zaman Wei Zhang Lei Zhang Weitao Zheng Xiaoqiang Cui State Key laboratory of Automotive Simulation and Control School of Materials Science and EngineeringKey Laboratory of Automobile Materials of MOEJilin Provincial International Cooperation Key Laboratory of High-Efficiency Clean Energy MaterialsElectron Microscopy CenterJilin UniversityChangchun 130012China College of Chemistry Jilin UniversityChangchun 130012China

Designing high-performance electrocatalysts toward hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)is essential to reduce the activation barrier and optimize free adsorption energy of reactive intermediates.Herein,we report that incorporating high-valence Cr into NiSe_(2)(Cr_(x)Ni_(1-x)Se_(2))kinetically and thermodynamically expedites elementary steps of both HER and OER.The as-prepared Cr_(0.05)Ni_(0.95)Se_(2) catalyst displays excellent HER and OER activities,with low overpotentials of 89 and 272 mV at the current density of 10 mA·cm^(-2)(j10),respectively,and remains stable during operation for 30 h.A low cell voltage of only 1.59 V is required to drive j10 in alkaline media.In situ Raman spectroscopy reveals that Cr incorporation facilitates the formation of NiOOH active species during the OER process.Meanwhile,theoretical explorations demonstrate that high-valence Cr incorporation efficiently accelerates water dissociation kinetics and improves H*adsorption during HER process,lowering the activation barrier of OER and optimizing the adsorption energy of oxygen-based intermediate,thus kinetically and thermodynamically enhancing the intrinsic performance of NiSe_(2) for over water splitting.This strategy provides a new horizon to design transition metal based electrocatalysts in the clean energy field.

关键词： nickel selenide electrocatalytic water splitting high-valence Cr density functional theory(DFT)calculation

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General synthesis of transition metal nitride arrays by ultrafast flash Joule heating within 500 ms

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Science China Chemistry 2024年第6期67卷 1976-1982页

作者： Peiqi Shen Jiahui Zhao Yanan Gao Yunxiang Lin Yuchen Han Kun Xu School of Chemistry and Chemical Engineering Key Laboratory of Functional Inorganic Material Chemistry of Anhui ProvinceAnhui Province Key Laboratory of Chemistry for Inorganic/Organic Hybrid Functionalized MaterialsKey Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of EducationAnhui UniversityHefei230601China Institutes of Physical Science and Information Technology Center of Free Electron Laser&High Magnetic FieldLeibniz International Joint Research Center of Materials Sciences of Anhui ProvinceAnhui UniversityHefei230601China

Transition metal nitrides(TMNs)are considered as viable alternatives to noble metal catalysts owing to their versatile electronic structure and favorable catalytic performance.However,the conventional synthetic processes for TMNs suffer from high energy consumption and low production yield.In this study,a range of TMNs and their hetero-composite arrays were successfully synthesized via an ultrafast flash Joule heating technology within 0.5 s.As a proof concept,the nitrides and hetero-composites were applied for the electrocatalytic hydrazine oxidation reaction(HzOR),in which the Co_(4)N/Mo_(16)N_(7)arrays shows the best performance with a geometric current density of 100 mA cm^(-2)at 23 mV(vs.reversible hydrogen electrode(RHE)).This work paves a new way for the ultrafast synthesis of TMNs which could meet the ever-increased energy crisis.

关键词： flash Joule heating rapid synthesis transition metal nitrides hydrazine oxidation reaction electrocatalysts

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Engineering Strategies for Suppressing the Shuttle Effect in Lithium–Sulfur Batteries

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Nano-Micro Letters 2024年第1期16卷 187-221页

作者： Jiayi Li Li Gao Fengying Pan Cheng Gong Limeng Sun Hong Gao Jinqiang Zhang Yufei Zhao Guoxiu Wang Hao Liu joint international laboratory On Environmental and Energy Frontier materials School of Environmental and Chemical EngineeringShanghai UniversityShanghaiPeople’s Republic of China Centre for Clean Energy Technology University of Technology SydneyBroadwaySydneyNSW 2007Australia

Lithium–sulfur(Li–S)batteries are supposed to be one of the most potential next-generation batteries owing to their high theoretical capacity and low cost.Nevertheless,the shuttle effect of firm multi-step two-electron reaction between sulfur and lithium in liquid electrolyte makes the capacity much smaller than the theoretical value.Many methods were proposed for inhibiting the shuttle effect of polysulfide,improving corresponding redox kinetics and enhancing the integral performance of Li–S batteries.Here,we will comprehensively and systematically summarize the strategies for inhibiting the shuttle effect from all components of Li–S batteries.First,the electrochemical principles/mechanism and origin of the shuttle effect are described in detail.Moreover,the efficient strategies,including boosting the sulfur conversion rate of sulfur,confining sulfur or lithium polysulfides(LPS)within cathode host,confining LPS in the shield layer,and preventing LPS from contacting the anode,will be discussed to suppress the shuttle effect.Then,recent advances in inhibition of shuttle effect in cathode,electrolyte,separator,and anode with the aforementioned strategies have been summarized to direct the further design of efficient materials for Li–S batteries.Finally,we present prospects for inhibition of the LPS shuttle and potential development directions in Li–S batteries.

关键词： Shuttle effect Designed strategies Li-S battery Lithium polysulfides

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Interface engineering strategy via electron-defect trimethyl borate additive toward 4.7 V ultrahigh-nickel LiNi_(0.9)Co_(0.05)Mn_(0.05)O_(2)battery

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Journal of Energy Chemistry 2024年第5期92卷 639-647页

作者： Yilin Zhang Yuqing Chen Qiu He Jinlong Ke Wei Wang Jian-Fang Wu Peng Gao Yanhua Li Jilei Liu College of materials Science and Engineering Hunan Joint International Laboratory of Advanced Materials and Technology for Clean EnergyHunan Province Key Laboratory for Advanced Carbon Materials and Applied TechnologyHunan UniversityChangsha 410082HunanChina College of materials Science and Engineering Sichuan UniversityChengdu 610065SichuanChina School of materials Science and Engineering Hunan Institute of TechnologyHengyang 421002HunanChina

The Li metal battery with ultrahigh-nickel cathode(LiNi_(x)M_(1-x)O_(2),M=Mn,Co,and x≥0.9)under high-voltage is regarded as one of the most promising approaches to fulfill the ambitious target of 400 Wh/kg.However,the practical application is impeded by the instability of electrode/electrolyte interface and Ni-rich cathode itself.Herein we proposed an electron-defect electrolyte additive trimethyl borate(TMB)which is paired with the commercial carbonate electrolyte to construct highly conductive fluorine-and boron-rich cathode electrolyte interface(CEI)on LiNi_(0.9)Co_(0.05)Mn_(0.05)O_(2)(NCM90)surface and solid electrolyte interphase(SEI)on lithium metal surface.The modified CEI effectively mitigates the structural transformation from layered to disordered rock-salt phase,and consequently alleviate the dissolution of transition metal ions(TMs)and its“cross-talk”effect,while the enhanced SEI enables stable lithium plating/striping and thus demonstrated good compatibility between electrolyte and lithium metal anode.As a result,the common electrolyte with 1 wt%TMB enables 4.7 V NCM90/Li cell cycle stably over 100 cycles with 70%capacity retention.This work highlights the significance of the electron-defect boron compounds for designing desirable interfacial chemistries to achieve high performance NCM90/Li battery under high voltage operation.

关键词： NCM90 batteries Electrolyte additive Trimethyl borate

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Dynamic Control of Multiple Optical Patterns of Cholesteric Liquid Crystal Microdroplets by Light-Driven Molecular Motors

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CCS Chemistry 2024年第2期6卷 427-438页

作者： Jiaqin Li Shuting Xie Jiahui Meng Yuying Liu Qi Zhan Yang Zhang Lingling Shui Guofu Zhou Ben L.Feringa Jiawen Chen SCNU-UG international joint laboratory of Molecular Science and Displays National Center for International Research on Green OptoelectronicsSouth China Normal UniversityGuangzhou 510006 joint laboratory of Optofluidic Technology and systems Guangdong Provincial Key Laboratory of Nanophotonic Functional Materials and DevicesSchool of Information and Optoelectronic Science and EngineeringSouth China Normal UniversityGuangzhou 510006 Stratingh Institute for Chemistry University of Groningen9747AG Groningen

The key to high-level encryption and anti-counterfeiting techniques is the storage of multiple levels of distinct information that can be individually and precisely addressed by certain stimuli.This continues to be a formidable challenge as the concealed images or codes must be read with fast response and high resolution without cross-talk to the first layer of information.Here,we report a non-fluorescencebased strategy to establish responsive encryption labels taking advantage of solely tuning multiple optical patterns of cholesteric liquid crystal(CLC)microdroplets doped with light-driven molecular motors.The photo-triggered unidirectional rotation of the motor induced not only changes in the helical twist power value but the opposite helical orientation of the superstructure in CLCs as well,resulting in changes in both the structural color and the selective reflection of circularly polar light.The designed labels,which featured highly selective addressability of dual-level distinct information,good reversibility,and viewing angle-independence,were applied to build devices for daily practical use,demonstrating great potential in anti-counterfeiting technology and provide a versatile platform for enhanced data protection and encryption of authentic information.

关键词： molecular motor chirality amplification cholesteric liquid crystal anti-counterfeiting label data encryption

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In situ calibrated angle between the quantization axis and the propagating direction of the light field for trapping neutral atoms

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Chinese Physics B 2024年第2期33卷 318-323页

作者：郭瑞军何晓东盛诚王坤鹏许鹏刘敏王谨孙晓红曾勇詹明生 Henan Key laboratory of Laser and Optoelectronic Information National Center for International Joint Research of Electronic Materials and SystemsSchool of Electrical and Information EngineeringZhengzhou UniversityZhengzhou 450001China State Key laboratory of Magnetic Resonance and Atomic and Molecular Physics Innovation Academy for Precision Measurement Science and TechnologyChinese Academy of SciencesWuhan 430071China

The recently developed magic-intensity trapping technique of neutral atoms efficiently mitigates the detrimental effect of light shifts on atomic qubits and substantially enhances the coherence time. This technique relies on applying a bias magnetic field precisely parallel to the wave vector of a circularly polarized trapping laser field. However, due to the presence of the vector light shift experienced by the trapped atoms, it is challenging to precisely define a parallel magnetic field, especially at a low bias magnetic field strength, for the magic-intensity trapping of85Rb qubits. In this work, we present a method to calibrate the angle between the bias magnetic field and the trapping laser field with the compensating magnetic fields in the other two directions orthogonal to the bias magnetic field direction. Experimentally, with a constantdepth trap and a fixed bias magnetic field, we measure the respective resonant frequencies of the atomic qubits in a linearly polarized trap and a circularly polarized one via the conventional microwave Rabi spectra with different compensating magnetic fields and obtain the corresponding total magnetic fields via the respective resonant frequencies using the Breit–Rabi formula. With known total magnetic fields, the angle is a function of the other two compensating magnetic fields.Finally, the projection value of the angle on either of the directions orthogonal to the bias magnetic field direction can be reduced to 0(4)° by applying specific compensating magnetic fields. The measurement error is mainly attributed to the fluctuation of atomic temperature. Moreover, it also demonstrates that, even for a small angle, the effect is strong enough to cause large decoherence of Rabi oscillation in a magic-intensity trap. Although the compensation method demonstrated here is explored for the magic-intensity trapping technique, it can be applied to a variety of similar precision measurements with trapped neutral atoms.

关键词： quantization axis trapping laser angle compensating magnetic fields

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Heterostructured Pt-Ni_(3)Mo_(3)N formed via ammonia-containing polyoxometalates for highly efficient electrocatalytic hydrogen evolution in acid medium

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Journal of Energy Chemistry 2024年第5期92卷 698-704页

作者： Bianqing Ren Xue Gong Jing Cao Dezheng Zhang Zizhun Wang Ping Song Ce Han Weilin Xu State Key laboratory of Electroanalytical Chemistry Jilin Province Key Laboratory of Low Carbon Chemical PowerChangchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022JilinChina School of Applied Chemistry and Engineering University of Science and Technology of ChinaHefei 230026AnhuiChina Key laboratory of Automobile materials MOE School of Materials Science&EngineeringJilin Provincial International Cooperation Key Laboratory of High-Efficiency Clean Energy MaterialsElectron Microscopy Centerand International Center of Future ScienceJilin UniversityChangchun 130012JilinChina

Constructing heterostructured nanohybrid is considered as a prominent route to fabricate alternative electrocatalysts to commercial Pt/C for hydrogen evolution reaction(HER).In this work,(NH_(4))_(4)[NiH_(6)Mo_(6)O_(4)]·5H_(2)O polyoxometalates(NiMo_(6))are adopted as the cluster precursors for simple fabrication of heterostructured Pt-Ni_(3)Mo_(3)N nanohybrids supported by carbon black(Pt-Ni_(3)Mo_(3)N/C)without using additional N sources.The improved porosity and enhanced electronic interaction of Pt-Ni_(3)Mo_(3)N/C should be attributed to the integration of Pt with NiMo_(6),which favors the mass transport,promotes the formation of exposed catalytic sites,and benefits the regulation of intrinsic activity.Thus,the as-obtained Pt-Ni_(3)Mo_(3)N/C exhibits impressive and durable HER performance as indicated by the low overpotential of 13.7 mV at the current density of 10 mA cm^(-2) and the stable overpotential during continuous working at 100 mA cm^(-2) for 100 h.This work provides significant insights for the synthesis of new highly active heterostructured electrocatalysts for renewable energy devices.

关键词： Polyoxometalates Cluster precursors Heterostructured nanohybrids Hydrogen evolution reaction Electrocatalysis

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