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Efficient ORR catalysts for zinc-air battery: Biomass-derived ultra-stable co nanoparticles wrapped with graphitic layers via optimizing electron transfer

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Journal of Energy Chemistry 2022年第7期31卷 211-218,I0006页

作者： Yu Feng Kexin Song Wei Zhang Xinyan Zhou Seung Jo Yoo Jin-Gyu Kim Sifan Qiao Yugang Qi Xu Zou Zhongjun Chen Tingting Qin Nailin Yue Zizhun Wang Dabing Li Weitao Zheng State Key Laboratory of Automotive Simulation and control School of Materials Science&EngineeringKey Laboratory of Automobile Materials MOEElectron Microscopy Centerand International Center of Future ScienceJilin UniversityJilin UniversityChangchun 130012JilinChina Division of Scientific Instrumentation&Management Korea Basic Science InstituteDaejeon 34133Republic of Korea Institute of High Energy Physics Chinese Academy of SciencesBeijing 100049China State Key Laboratory of Luminescence and Applications Changchun Institute of OpticsFine Mechanics and PhysicsChinese Academy of SciencesChangchun 130033JilinChina

The poor stability of non-noble metal catalysts in oxygen reduction reaction(ORR) is a main bottleneck that limits their big-scale application in metal-air batteries. Herein, we construct a chainmail catalyst(co-NC-AD) with outstanding stability, via the competitive complexation and post absorption strategy,consisting of highly graphitic layers wrapped uniform-size co nanoparticles(co-NPs). Experiments combined with density functional theory(DFT) calculations jointly confirmed that the electron transfer occurred from the inner co-NPs to the external graphitic layers. It facilitated the adsorption process of oxygen molecules and the hybridization of the O-2 p and C-1 p orbitals, which accelerated the ORR reaction kinetics. consequently, our prepared co-NC-AD shows excellent ORR activity, offered with a more positive initial potential(E_(onset)= 0.95 V) and half-wave potential(E_(1/2)= 0.86 V). The remarkable stability and resistance of methanol poisoning are merited from the protection effect of stable graphitic layers. In addition, the high electrochemical performance of co-NC-AD-based zinc-air battery demonstrates their potential for practical applications. Therefore, our work provides new ideas for the design of nanoconfined catalysts with high stability and activity.

关键词： Chainmail catalyst Graphitic layers co nanoparticles Oxygen reduction reaction

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Tailoring structural properties of carbon via implanting optimal co nanoparticles in n-rich carbon cages toward high-efficiency oxygen electrocatalysis for rechargeable zn-air batteries

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Carbon Energy 2022年第4期4卷 576-585页

作者： Jie Yu Yawen Dai Zhenbao Zhang Tong Liu Siyuan Zhao Chun Cheng Peng Tan Zongping Shao Meng Ni Department of Building and Real Estate The Hong Kong Polytechnic UniversityKowloonHong KongChina Department of Thermal Science and Energy Engineering University of Science and Technology of ChinaHefeiAnhuiChina State Key Laboratory of Materials-Oriented Chemical Engineering Department of Chemical EngineeringCollege of Chemical EngineeringNanjing Tech UniversityNanjingChina Department of Chemical Engineering Curtin UniversityPerthWestern AustraliaAustralia

Rational construction of carbon-based materials with high-efficiency bifunctionality and low cost as the substitute of precious metal catalyst shows a highly practical value for rechargeable Zn-air batteries(ZABs)yet it still remains challenging.Herein,this study employs a simple mixing-calcination strategy to fabricate a high-performance bifunctional composite catalyst composed of N-doped graphitic carbon encapsulating co nanoparticles(co@NrC).Benefiting from the core-shell architectural and compositional advantages of favorable electronic configuration,more exposed active sites,sufficient electric conductivity,rich defects,and excellent charge transport,the optimal co@NrC hybrid(co@NrC-0.3)presents outstanding catalytic activity and stability toward oxygen-related electrochemical reactions(oxygen reduction and evolution reactions,i.e.,ORR and OER),with a low potential gap of 0.766 V.Besides,the rechargeable liquid ZAB assembled with this hybrid electrocatalyst delivers a high peak power density of 168 mW cm^(−2),a small initial discharge-charge potential gap of 0.45 V at 10 mA cm^(−2),and a good rate performance.Furthermore,a relatively large power density of 108 mW cm^(−2) is also obtained with the co@NrC-0.3-based flexible solid-state ZAB,which can well power LED lights.Such work offers insights in developing excellent bifunctional electrocatalysts for both OER and ORR and highlights their potential applications in metal-air batteries and other energy-conversion/storage devices.

关键词： co nanoparticles core-shell nanostructure N-doped graphitic carbon oxygen electrocatalysis Zn-air battery

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Ultralong nitrogen/sulfur co-doped carbon nano-hollowsphere chains with encapsulated cobalt nanoparticles for highly efficient oxygen electrocatalysis

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Carbon Energy 2023年第8期5卷 15-30页

作者： Wei Zhang Xingmei Guo cong Li Jiang-Yan Xue Wan-Ying Xu Zheng Niu Hongwei Gu Carl Redshaw Jian-Ping Lang college of Chemistry Chemical Engineering and Materials ScienceSoochow UniversitySuzhouChina State Key Laboratory of Organometallic Chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghaiChina college of Environmental and Chemical Engineering Jiangsu University of Science and TechnologyZhenjiangChina Department of Chemistry University of HullHullUK

The development of simple and effective strategies to prepare electrocatalysts,which possess unique and stable structures comprised of metal/nonmetallic atoms for oxygen reduction reaction(ORR)and oxygen evolution reaction(OER),is currently an urgent issue.Herein,an efficient bifunctional electrocatalyst featured by ultralong N,S-doped carbon nano-hollow-sphere chains about 1300 nm with encapsulated co nanoparticles(co-CNHSCs)is developed.The multifunctional catalytic properties of co together with the heteroatom-induced charge redistribution(i.e.,modulating the electronic structure of the active site)result in superior catalytic activities toward OER and ORR in alkaline media.The optimized catalyst co-CNHSC-3 displays an outstanding electrocatalytic ability for ORR and OER,a high specific capacity of 1023.6 mAh gZn^(-1),and excellent reversibility after 80 h at 10mA cm^(-2)in a Zn-air battery system.This work presents a new strategy for the design and synthesis of efficient multifunctional carbon-based catalysts for energy storage and conversion devices.

关键词： co nanoparticles N S co-doping oxygen electrocatalysts rechargeable Zn-air batteries ultralong carbon nano-hollow-sphere chains

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cobalt-nanoparticle catalysts derived from zeolitic imidazolate framework@MXene composites for efficient oxidative self-coupling of benzylamines

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Frontiers of Chemical Science and Engineering 2024年第1期18卷 95-106页

作者： Jie Chen Mingyuan Jian Deqiong Xie Kecan Dou Deli Chen Weidong Zhu Fumin Zhang Key Laboratory of the Ministry of Education for Advanced Catalysis Materials Institute of Physical ChemistryZhejiang Normal UniversityJinhua 321004China

In this study,we synthesize a catalyst comprising cobalt nanoparticles supported on MXene by pyrolyzing a composite in a N2 environment.Specifically,the composite comprises a bimetallic Zn/co zeolitic imidazole framework grown in situ on the outer surface of MXene.The catalytic efficiency of the catalyst is tested for the self-coupling of 4-methoxybenzylamine to produce value-added imine,where atmospheric oxygen(1 atm)is used as the oxidant.Based on the results,the catalyst displayed impressive catalytic activity,achieving 95.4%yield of the desired imine at 383 K for 8 h.Furthermore,the catalyst showed recyclability and tolerance toward benzylamine substrates with various functional groups.The outstanding performance of the catalyst is primarily attributed to the synergetic catalytic effect between the cobalt nanoparticles and MXene support,while also benefiting from the three-dimensional porous structure.Additionally,a preliminary investigation of potential reaction mechanisms is conducted.

关键词： MXene sacrificial template oxidative self-coupling co nanoparticles imine

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Highly active and stable co nanoparticles embedded in nitrogen-doped mesoporous carbon nanofibers for aqueous-phase levulinic acid hydrogenation

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Green Energy & Environment 2021年第4期6卷 567-577页

作者： Shuai Shao Ying Yang Shangwei Guo Shijie Hao Feng Yang Suoying Zhang Yang Ren Yangchuan Ke State Key Laboratory of Heavy Oil Processing China University of PetroleumChangpingBeijing102249China X-Ray Science Division Argonne National Laboratory9700 S.Cass Ave.ArgonneIllinois60439USA

Developing a highly active and durable non-noble metal catalyst for aqueous-phase levulinic acid(LA)hydrogenation to g-valerolactone(GVL)is an appealing yet challenging task.Herein,we report well-dispersed co nanoparticles(NPs)embedded in nitrogen-doped mesoporous carbon nanofibers as an efficient catalyst for aqueous-phase LA hydrogenation to GVL.The co zeolitic imidazolate framework(ZIF-67)nanocrystals were anchored on the sodium dodecyl sulfate modified wipe fiber(WF-S),yielding one-dimensional(1-D)structured composite(ZIF-67/WF-S).Subsequently,co NPs were uniformly embedded in nitrogen-doped mesoporous carbon nanofibers(co^(R)NC/SMCNF)through a pyrolysis-reduction strategy using ZIF-67/WF-S as the precursor.Benefiting from introducing modified wipe fiber WF-S to enhance the dispersion of co NPs,and co^(0) with co-N_xdual active sites,the resulting co^(R)NC/SMCNF catalyst shows brilliant catalytic activity(206 h^(-1) turnover frequency).Additionally,the strong metal-support interactions greatly inhibited the co NPs from aggregation and leaching from the mesoporous carbon nanofibers,and thus increasing the reusability of the co^(R)NC/SMCNF catalyst(reusable nine times without notable activity loss).

关键词： co nanoparticles Mesoporous carbon nanofiber Dual active sites Aqueous levulinic acid hydrogenation High stability

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converting co^(2+)-impregnated g-C_(3)N_(4) into N-doped CNTs-confined co nanoparticles for efficient hydrogenation rearrangement reactions of furanic aldehydes

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Nano Research 2021年第8期14卷 2846-2852页

作者： Dongdong Wang Mohammad Al-Mamun Wanbing Gong Yang Lv Chun Chen Yue Lin Guozhong Wang Haimin Zhang Huijun Zhao Key Laboratory Centre for Environmental and Energy NanomaterialsAnhui Key Laboratory of Nanomaterials and NanotechnologyCAS Centre for Excellence in NanoscienceInstitute of Solid State PhysicsChinese Academy of SciencesHefei 230031China University of Science and Technology of China Hefei 230026China Centre for Clean Environment and Energy Gold Coast CampusGriffith UniversityQueensland 4222Australia Hefei National Laboratory for Physical Sciences at the Microscale University of Science and Technology of ChinaHefei 230026China

The cyclopentanone and derivatives are a class of crucial fine chemicals for various industries and currently produced by conventional petrochemical synthetic routes.Here,we demonstrated a new synthetic approach to directly fabricate N-doped carbon nanotube(N-CNTs)networks with confined co nanoparticles from co^(2+)-impregnated bulk g-C_(3)N_(4) as high performance hydrogenation rearrangement(HR)catalyst to efficiently convert a wide spectrum of biomass-derived furanic aldehydes to the corresponding cyclopentanones in water under a record-low H2 pressure of 0.5 MPa and mild temperature.We unveiled a co-catalysed bulk g-C_(3)N_(4) decomposition/carbonisation CNTs formation mechanism.A new HR pathway was also unveiled.

关键词： g-C_(3)N_(4) co nanoparticles carbon nanotubes hydrogenation rearrangement furanic aldehydes

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“Charging”the cigarette butt:heteroatomic porous carbon nanosheets with edge-induced topological defects for enhanced oxygen evolution performance

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Frontiers of Chemical Science and Engineering 2023年第11期17卷 1755-1764页

作者： Qing-Hui Kong Xian-Wei Lv Jin-Tao Ren Hao-Yu Wang Xin-Lian Song Feng Xu Zhong-Yong Yuan School of Materials Science and Engineering Smart Sensing Interdisciplinary Science CenterNankai UniversityTianjin 300350China Tianjin Workstation Technology Center of Shanghai Tobacco Group Co.Ltd.Tianjin 300163China Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education) Nankai UniversityTianjin 300071China

Owing to the complexity of electron transfer pathways,the sluggish oxygen evolution reaction process is defined as the bottleneck for the practical application of Zn-air batteries.In this effort,metal nanoparticles(co,Ni,Fe,etc.)encapsulated within nitrogen-doped carbon materials with abundant edge sites were synthesized by one-step pyrolysis treatment using cigarette butts as raw materials,which can drastically accelerate the overall rate of oxygen evolution reaction by facilitating the adsorption of oxygenated intermediates by the edge-induced topological defects.The prepared catalyst of nitrogen-doped carbon porous nanosheets loaded with co nanoparticles(co@NC-500)exhibits enhanced catalytic activity toward oxygen evolution reaction,with a low overpotential of 350 mV at the current density of 10 mA·cm^(-2).Furthermore,the Zn-air battery assembled with co@NC-500 catalyst demonstrates a desirable performance affording an open-circuit potential of 1.336 V and power density of 33.6 mW·cm^(-2),indicating considerable practical application potential.

关键词： oxygen evolution reaction porous carbon nanosheets co nanoparticles edge-induced topological defects Zn-air batteries

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Highly Dispersive co@N-C Catalyst as Freestanding Bifunctional Cathode for Flexible and Rechargeable Zinc–air Batteries

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Energy & Environmental Materials 2022年第2期5卷 543-554页

作者： Yu Ma Ding Chen Weijun Li Yapeng Zheng Lin Wang Gang Shao Qiao Liu Weiyou Yang college of Materials Science and Engineering Hunan UniversityChangsha 410082China State Key Laboratory of Advanced Design and Manufacturing for Vehicle Body College of Mechanical and Vehicle EngineeringHunan UniversityChangsha 410082China Institute of Materials Ningbo University of TechnologyNingbo 315211China School of Materials Science and Engineering Zhengzhou UniversityZhengzhou 450001China

The design of efficient cathode with great cycle performance,high flexibility,and low cost is essential for the commercialization of zinc–air battery(ZAB).Herein,we report the exploration of freestanding bifunctional cathode with rationally designed structures,namely,tiny co nanoparticles embedded in Ndoped carbon nanofiber aerogels,which have desired features including uniform co dispersity,balanced distribution of N-C species,hierarchically porous structure with increased fraction of meso-to micropores,and moderate amounts of defects.Accordingly,the as-fabricated cathodes exhibit positive half-wave potential of 0.82 V for oxygen reduction and small overpotential of 350 mV at 10 mA cm^(−2) for oxygen evolution,respectively,which deliver smaller reversible oxygen electrode index(0.76 V)than the commercial Pt/C+RuO_(2)(0.80 V)and most co-based electrocatalysts ever reported.Impressively,the as-constructed liquid rechargeable ZAB behaves high peak power density(160 mW cm^(−2)),large specific capacity(759.7 mAh g^(−1) at 10 mA cm^(−2),tested after 120 h of OCV tests),and robust stability over 277 h.Moreover,the as-assembled quasi-solid-state ZAB using such freestanding cathode represents excellent mechanical flexibility and outstanding cycle performance,regardless of being serviced under extremely bending conditions from 0°to 180°,underscoring their promising applications as durable bifunctional cathode for portable metalair batteries.

关键词： bifunctional cathode carbon nanofiber aerogels co nanoparticles freestanding cathode zinc-air batteries

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Graphene-supported cobalt nanoparticles used to activate SiO_(2)-based anode for lithium-ion batteries

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Chinese Chemical Letters 2023年第3期34卷 447-453页

作者： Qi An Xiaohong Sun Ying Na Shu Cai Chunming Zheng School of Materials Science and Engineering Key Laboratory of Advanced Ceramics and Machining Technology of Ministry of EducationTianjin UniversityTianjin 300072China School of Chemistry and Chemical Engineering State Key Laboratory of Hollow-fiber Membrane Materials and Membrane ProcessesTiangong UniversityTianjin 300387China

Although SiO_(2)-based anode is a strong competitor to supersede graphite anode for lithium-ion batteries,it still has problems such as low electrochemical activity, enormous loss of active lithium, and serious volume expansion. In order to solve these problems, we used a graphene network loaded with cobalt metal nanoparticles(rGO-co) to coat SiO_(2) porous hollow spheres(SiO_(2)@rGO-co). The construction of porous hollow structure and graphene network can shorten the lithium-ion(Li^(+)) diffusion distance and enhance the conductivity of the composite, which improves the electrochemical activity of SiO_(2) effectively. They also alleviate the volume expansion of the anode in the cycling process. Moreover,nano-scale cobalt metal particles dispersed on graphene catalyze the conversion reaction of SiO_(2) and activate the locked Li+in Li_(2)O through a reversible reaction, which improves the charge and discharge capacity of the anode. The capacity of SiO_(2)@rGO-co reaches 370.4 m Ah/g after 100 cycles at 0.1 A/g,which is 6.19 times the capacity of pure SiO_(2)(59.8 mAh/g) under the same circumstance. What is more,its structure also exhibits excellent cycle stability, with a volume expansion rate of only 13.0% after 100 cycles at a current density of 0.1 A/g.

关键词： Lithium-ion batteries SiO_(2)-based anode Graphene network co nanoparticles Electrochemical activity

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Efficient Catalytic conversion of Polysulfides by Biomimetic Design of “Branch‑Leaf” Electrode for High‑Energy Sodium–Sulfur Batteries

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Nano-Micro Letters 2021年第3期13卷 155-167页

作者： Wenyan Du Kangqi Shen Yuruo Qi Wei Gao Mengli Tao Guangyuan Du Shu‑juan Bao Mingyang Chen Yuming Chen Maowen Xu Key Laboratory of Luminescence Analysis and Molecular Sensing(Southwest University) Ministry of EducationSchool of Materials and EnergySouthwest UniversityChongqing 400715People’s Republic of China Beijing computational Science Research Center Beijing 100193People’s Republic of China Center for Green Innovation School of Materials Science and EngineeringUniversity of Science and Technology BeijingBeijing 100083People’s Republic of China college of Environmental Science and Engineering Fujian Normal UniversityFuzhou 350007People’s Republic of China

Rechargeable room temperature sodium–sulfur(RT Na–S)batteries are seriously limited by low sulfur utilization and sluggish electrochemical reaction activity of polysulfide intermediates.Herein,a 3D“branch-leaf”biomimetic design proposed for high performance Na–S batteries,where the leaves constructed from co nanoparticles on carbon nanofibers(CNF)are fully to expose the active sites of co.The CNF network acts as conductive“branches”to ensure adequate electron and electrolyte supply for the co leaves.As an effective electrocatalytic battery system,the 3D“branch-leaf”conductive network with abundant active sites and voids can effectively trap polysulfides and provide plentiful electron/ions pathways for electrochemical reaction.DFT calculation reveals that the co nanoparticles can induce the formation of a unique co–S–Na molecular layer on the co surface,which can enable a fast reduction reaction of the polysulfides.Therefore,the prepared“branch-leaf”CNF-L@co/S electrode exhibits a high initial specific capacity of 1201 mAh g^−1 at 0.1 C and superior rate performance.

关键词： co nanoparticles Sodium-sulfur batteries Branch-leaf,biomimetic

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