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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 ***,we report well-dispersed co nanoparticles(NPs)embedded in nitrogen-doped mesoporous carbon nanofibers as an efficient catalyst for aqueous-phase LA hydrogenation to *** 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 *** 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

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

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 ***,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 *** 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

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 ***,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 ***,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 ***,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 *** 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

Promoting reaction kinetics of lithium polysulfides by cobalt polyphthalocyanine derived ultrafine co nanoparticles mono-dispersed on graphene flakes for Li-S batteries

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Journal of Central South University 2022年第9期29卷 2940-2955页

作者： CHEN Xia ZHOU Jiang-qi XIAO Zi-chun HAN Ting-ting ZHOU Ya-nan CHEN Qi-ming TANG Wei School of Chemical Engineering and Technology Xi’an Jiaotong UniversityXi’an 710049China State Key Laboratory of Space Power-sources Technology Shanghai Institute of Space Power-SourcesShanghai 200245China

Lithium-sulfur(Li-S)batteries have been considered as the next generation high energy storage ***,its commercialization has been hindered by several issues,especially the dissolution and shuttle of the soluble lithium polysulfides(LiPSs)as well as the slow reaction kinetics of LiPSs which may make shuttling effect even ***,we report a strategy to address this issue by in-situ transformation of co−N_(x) coordinations in cobalt polyphthalocyanine(coPPc)into co nanoparticles(co NPs)embedded in carbon matrix and mono-dispersed on graphene *** co NPs can provide rich binding and catalytic sites,while graphene flakes act as ideally LiPSs transportation and electron conducting *** a remarkable enhanced reaction kinetics of LiPSs via these merits,the sulfur host with a sulfur content up to 70 wt%shows a high initial capacity of 1048 mA∙h/g at 0.2C,good rate capability up to 399 mA·h/g at 2C.

关键词： cobalt polyphthalocyanine co nanoparticles binding-sites catalytic-conversion shuttle-effect Li-S batteries

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 ***,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 *** 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 *** 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 *** 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

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 ***,the composite comprises a bimetallic Zn/co zeolitic imidazole framework grown in situ on the outer surface of *** 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 *** on the results,the catalyst displayed impressive catalytic activity,achieving 95.4%yield of the desired imine at 383 K for 8 ***,the catalyst showed recyclability and tolerance toward benzylamine substrates with various functional *** 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 ***,a preliminary investigation of potential reaction mechanisms is conducted.

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

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 ***,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 *** CNF network acts as conductive“branches”to ensure adequate electron and electrolyte supply for the co *** 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 *** 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 ***,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

A highly selective catalyst of co/La_(4)Ga_(2)O_(9) for co_(2) hydrogenation to ethanol

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Journal of Energy Chemistry 2021年第5期30卷 486-495页

作者： Kang An Siran Zhang Jiaming Wang Qiang Liu Ziyang Zhang Yuan Liu Department of Catalysis Science and Technology School of Chemical EngineeringTianjin UniversityTianjin 300350China collaborative Innovation Center of Chemical Science and Engineering(Tianjin) Tianjin 300072China

A new catalyst of co/La_(4)Ga_(2)O_(9) for co_(2) hydrogenation to produce ethanol was prepared by reducing Laco^(0).5 Ga0.5 O3,which showed excellent selectivity to ethanol(%35 C-mol%)at mild reaction conditions(270°C,3.5 MPa,3000 m L g-1 h-1).The catalysts were characterized by N_(2) adsorption/desorption,XRD,XAFS,co and co_(2)-TPD,H2 chemisorption,XPS and TEM *** interaction between co nanoparticles(NPs)and La2+4 Ga_(2)O_(9) oxide resulted in co^(0)-coon the surface of co *** was proposed that La_(4)Ga_(2)O_(9) could catalyze reverse water gas shift reaction(r-WGS),which converted co_(2) to ***,the co migrated to co^(0)-co^(2+)on co NPs,where it was hydrogenated to form ethanol like higher alcohols synthesis from *** results suggest that by controlling the oxidation state of cobalt,and combined with a kind of active site for activating co_(2) to form co,a catalyst with excellent selectivity to ethanol could be obtained for co_(2) hydrogenation,which means that the complex reaction may be proceed with high selectivity using only one active metal component.

关键词： co_(2)hydrogenation Ethanol synthesis Perovskite Gallium co nanoparticles

Elucidating the role of embedding dispersed cobalt sites in nitrogen-doped carbon frameworks in Si-based anodes for stable and superior storage

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Journal of Energy Chemistry 2024年第11期98卷 180-195页

作者： Yueying Chen Ping Li Mianying Huang Chunlei Wu Qianhong Huang Tingyang Xie Xiaoming Lin Akif Zeb Yongbo Wu Zhiguang Xu Yuepeng Cai Joint Laboratory of Energy and Materials Chemistry(South China Normal University-Guangzhou Tianci New Materials co.Ltd.) Key Laboratory of Theoretical Chemistry of EnvironmentMinistry of EducationSchool of ChemistrySouth China Normal UniversityGuangzhou 510006GuangdongChina Department of Chemistry and Chemical Engineering Jiangxi Normal UniversityNanchang 330022JiangxiChina Guangzhou Huifu Research Institute co.Ltd Nanxiang San LuGuangzhou 510663GuangdongChina Key Laboratory of Atomic and Subatomic Structure and Quantum control(Ministry of Education) Guangdong Basic Research Center of Excellence for Structure and Fundamental Interactions of MatterSchool of PhysicsSouth China Normal UniversityGuangzhou 510006GuangdongChina Guangdong Provincial Key Laboratory of Quantum Engineering and Quantum Materials Guangdong-Hong Kong Joint Laboratory of Quantum MatterSouth China Normal UniversityGuangzhou 510006GuangdongChina

Unsatisfactory conductivity and volume effects have hindered the commercial application of siliconbased materials as advanced anode materials for high-performance lithium-ion batteries. Herein, nitrogen doped carbon silicon matrix composite with atomically dispersed co sites(Si/co-N-C) is obtained via the design of the frame structure loaded with nano-components and the multi-element hybrid strategy. co atoms are uniformly fixed to the N-C frame and tightly packed with nanoscale silicon particles as an activation and protection building block. The mechanism of the N-C framework of loaded metal co in the Si alloying process is revealed by electrochemical kinetic analysis and ex situ characterization ***, the nitrogen-doped co site activates the intercalation of the outer carbon matrix to supplement the additional capacity. The co nanoparticles with high conductivity and support enhance the conductivity and structural stability of the composite, accelerating the Li^(+)/Na^(+) diffusion kinetics. Density functional theory(DFT) calculation confirms that the hetero-structure Si/co-N-C adjusts the electronic structure to obtain good lithium-ion adsorption energy, reduces the Li^(+)/Na^(+) migration energy *** work provides meaningful guidance for the development of high-performance metal/non-metal modified anode materials.

关键词： co nanoparticles Nitrogen doped carbon Silicon Lithium/sodium storage Metal-organic frameworks(MOFs)