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CCS Chemistry 2024年第10期6卷 2502-2514页

作者： Kang Huang Hao Wan Zhichao Gong Jianbin Liu Minmin Yan Jun Wu Chunyu Cui Gonglan Ye Karsten Reuter huilong fei Advanced Catalytic Engineering Research Center of the Ministry of Education State Key Laboratory for Chemo/Biosensing and ChemometricsCollege of Chemistry and Chemical EngineeringHunan UniversityChangsha 410082 Fritz-Haber-Institut der Max-Planck-Gesellschaft Berlin 14195

The formation of LiOH as the discharge product instead of Li_(2)O_(2)in Li-O_(2)batteries(LOBs)is highly desirable due to the associated drawbacks of Li_(2)O_(2)-based chemistry,which involves the generation of reactive oxygen intermediates responsible for substantial side ***,the current challenge lies in the formation pathway of LiOH,which typically requires the chemical hydrolysis of the hazardous LiO_(2)or Li_(2)O_(2)intermediate,posing risks to the battery ***,we report a direct 4e–electrochemical approach to LiOH enabled by a single atom catalyst(SAC)consisting of CoN_(3)moieties embedded in graphene(CoN_(3)-G),while Li_(2)O_(2)is formed on the metal-free nitrogen-doped graphene(NG).The direct 4e–LiOH pathway significantly reduces the parasitic reactions,resulting in negligible damage to the electrolyte and *** stands in strong contrast to the conventional 2e–Li_(2)O_(2)pathway mediated by NG and the indirect LiOH pathway by MnO_(2).Theoretical calculations further clarify that the presence of CoN_(3)sites enhances the adsorption of oxygen-containing intermediates like*OLiO and*Li_(2)O_(2),promoting the protonation of*Li_(2)O_(2)and the cleavage of the O–O bond to form *** work demonstrates a promising strategy to modulate the reaction pathways in LOBs and broadens the applications of SACs.

关键词： single atom catalyst LiOH Li-O_(2)batteries direct 4-electron oxygen reduction pathway selectivity

Aligned porous carbon film with ultralow loadings of Pt single atoms and clusters for high-current-density hydrogen generation

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Nano Research 2023年第1期16卷 256-263页

作者： Rui Liu Zhichao Gong Minmin Yan Gonglan Ye huilong fei Advanced Catalytic Engineering Research Center of the Ministry of Education State Key Laboratory for Chemo/Biosensing and Chemometricsand College of Chemistry and Chemical EngineeringHunan UniversityChangsha 410082China

The development of electrocatalysts toward the hydrogen evolution reaction(HER)with high-current-density capability is critical for the practical application of water splitting for hydrogen *** Pt-based materials are regarded as the most efficient HER catalysts,they suffer from scarcity and high ***,it is of vital importance to lower the loading of Pt while maintaining high ***,we report the fabrication of a monolithic aligned porous carbon film electrode co-modified with Pt single atoms and Pt nanoclusters(Pt SA/NC-AF)containing ultralow Pt content(0.038 wt.%)via a facile electrochemical deposition *** from the aligned porous structure of the carbon film and the high exposure of the Pt species,the optimized Pt SA/NCAF electrode exhibits outstanding HER performance in 0.5 M H_(2)SO_(4)with exceptional intrinsic activity(turnover frequency(TOF)=904.9 s^(−1)atη=100 mV)and ultrahigh mass activity(888.6 A·mg_(Pt)^(−1)atη=100 mV).Further,it can deliver an industrially relevant current density of 1,000 mA·cm−2 at an overpotential as low as 139 *** work provides a feasible avenue for the rational design of metal single-atom and nanocluster catalysts and additionally promotes the application of ultralow-loading noble metal-based catalysts in high-rate hydrogen production.

关键词： monolithic electrodes single atoms clusters hydrogen evolution reaction high current density

Ultrafast Joule heating synthesis of hierarchically porous graphene-based Co-N-C single-atom monoliths

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Nano Research 2022年第5期15卷 3913-3919页

作者： Lingli Xing Rui Liu Zhichao Gong Jingjing Liu Jianbin Liu Haisheng Gong Kang Huang huilong fei Advanced Catalytic Engineering Research Center of the Ministry of Education State Key Laboratory for Chemo/Biosensing and Chemometricsand College of Chemistry and Chemical EngineeringHunan UniversityChangsha 410082China

Herein,we develop a transient heating-quenching strategy triggered by Joule heating for the synthesis of single-atom cobalt-and nitrogen-doped graphene materials with three-dimensional porous monolithic architecture(denoted as CoNG-JH).The ultrafast Joule heating procedure simultaneously enables the reduction of graphene oxide and the incorporation of metal and nitrogen atoms into the graphene matrix within 2-second ***,the transient quenching avoids the extended heating-induced atom aggregation,ensuring the rapid and stable dispersion of atomic-scale CoNx active sites in ***,the interconnected macropores and nanopores formed by the self-assembly of graphene sheets facilitate the unimpeded ion and gas transport during the catalytic *** used as an electrode for the hydrogen evolution reaction(HER),the fabricated free-standing CoNG-JH exhibits high catalytic activity and durability with a low overpotential of 106 mV at 10 mA·cm^(-2) and a small Tafel slope of 66 mV·dec^(-1) in 0.5 M H_(2)SO_(4) *** presented synthesis and design strategy open up a rapid and facile route for the manufacturing of single atom catalysts.

关键词： Joule heating single atom catalysts hierarchically porous structure self-supporting film hydrogen evolution reaction

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“四位一体”的无机化学教学创新

大学化学 2024年第8期39卷 136-141页

作者：叶龚兰尹霞许峰杨鹏吴英鹏费慧龙湖南大学化学化工学院湖南大学化学

“无机化学”的授课对象为大一新生，学生的学业适应有待提高；课程的理论性强，理论与实验难以同步开展；同时，理论与实践不能有机融合。针对以上问题，为了提高拔尖学生的学习能力，教学团队进行了全面改革。依托信息化资源平台和人... 详细信息

“无机化学”的授课对象为大一新生，学生的学业适应有待提高；课程的理论性强，理论与实验难以同步开展；同时，理论与实践不能有机融合。针对以上问题，为了提高拔尖学生的学习能力，教学团队进行了全面改革。依托信息化资源平台和人工智能知识图谱，创新教学模式，通过混合式教学模式，解决部分学生学习与老师上课进度脱节的问题，提高学生自主学习能力并满足个性化需求；创新教学手段，将虚拟仿真等新技术引入课堂，解决理论与实验脱节的问题，提高学生深度学习能力；创新教学环境，依托学校实验平台和当地地质博物馆沉浸式学习，解决理论与实践脱节问题，提高学生实践创新能力；创新教学主导，依托博物馆，学生参与讲解员等志愿者活动，提高学生社会服务意识。“无机化学”的创新改革让课程平台资源更丰富、成果更多、教学质量获得同行高度认可，学生收益多、创新实践能力显著增强。

关键词：无机化学四位一体拔尖学生教学改革

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A High Capacity and Working Voltage Potassium-Based Dual Ion Batteries

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Energy & Environmental Materials 2021年第3期4卷 413-420页

作者： Meng Zhang Jiang Zhong Weiqing Kong Lei Wang Tao Wang huilong fei Haiyan Luo Jian Zhu Jiawen Hu Bingan Lu School of Chemistry and Chemical Engineering State Key Laboratory for Chemo/Biosensing and Chemometricsand College of ChemistryHunan UniversityChangsha 410082China School of Physics and Electronics Hunan UniversityChangsha 410082China

Potassium-based dual ion batteries(KDIBs)have attracted significant attention owing to high working voltage,high safety,low processing cost,and environmental ***,one great challenge for practical KDIBs is to develop suitable anode materials with high specific ***,we report an architecture of hierarchically porous antimony nanoparticles/carbon nanofibers(HPSb CNFs)as flexible,free-standing anode for high-performance *** HPSb CNFs with hierarchically porous structure,and high-content nitrogen doping,not only offer sufficient free space to tolerate the repetitive volume expansion of Sb nanoparticles during long-term cycling,but also greatly facilitate the transport of electrons and ions within electrode,ensuring high material utilization ***,the KDIBs,constituted by HPSb CNFs-700(calcined at 700°C)anode and graphite cathode,exhibited a high reversible capacity of 440 m Ah g^(-1)with high discharge medium voltage of 4.5 V at a specific current of 200 m A g^(-1)(the highest capacity for all KDIBs normalized by the mass of the anode),and excellent cyclic *** electrochemical reversibility of the KDIBs was further demonstrated by ex situ XRD,ex situ Raman spectrum,and *** results suggest the as-designed HPSb CNFs-700 with highcapacity and long-term cycling stability is a promising anode material for high-performance KDIBs.

关键词： antimony nanoparticles hierarchically porous structure high working voltage potassium dual ion batteries ultra-high capacity

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Hierarchically Micro/Nanostructured Current Collectors Induced by Ultrafast Femtosecond Laser Strategy for High-Performance Lithium-ion Batteries

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Energy & Environmental Materials 2022年第3期5卷 969-976页

作者： Yaya Wang Zexu Zhao Jiang Zhong Tao Wang Lei Wang Hanjiao Xu Jinhui Cao Jinhao Li Guanhua Zhang huilong fei Jian Zhu State Key Laboratory for Chemo/Biosensing and Chemometrics College of Chemistry and Chemical EngineeringHunan Key Laboratory of TwoDimensional MaterialsEngineering Research Center of Advanced CatalysisMinistry of EducationHunan UniversityChangsha 410082China State Key Laboratory of Advanced Design and Manufacturing for Vehicle Body Hunan Provincial Key Laboratory of Intelligent Laser ManufacturingHunan UniversityChangsha 410082China College of Mechanical and Vehicle Engineering Hunan UniversityChangsha 410082China

Commercial Cu and Al current collectors for lithium-ion batteries(LIBs)possess high electrical conductivity,suitable chemical and electrochemical ***,the relatively flat surface of traditional current collectors causes weak bonding strength and poor electrochemical contact between current collectors and electrode materials,resulting in potential detachment of active materials and rapid capacity degradation during extended ***,we report an ultrafast femtosecond laser strategy to manufacture hierarchical micro/nanostructures on commercial Al and Cu foils as current collectors for high-performance *** hierarchically micro/nanostructured current collectors(HMNCCs)with high surface area and roughness offer strong adhesion to active materials,fast electronic delivery of entire electrodes,significantly improving reversible capacities and cyclic stability of HMNCCs based ***,LiNi_(0.5)Co_(0.2)Mn_(0.3)O_(2)(NCM523)cathode with Al HMNCC generated a high reversible capacity after 200 cycles(25%higher than that of cathode with Al CC).Besides,graphite anode with Cu HMNCC also maintained prominent reversible capacity even after 600 ***,the full cell assembled by graphite anode with Cu HMNCC and NCM523 cathode with Al HMNCC achieved high reversible capacity and remarkable cycling stability under industrial-grade mass *** study provides promising candidate for achieving high-performance LIBs current collectors.

关键词： currentcollectors femtosecondlaserstrategy hierarchical micro/nanostructures high rate performance lithium-ion battery

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Sandwich structured graphene-wrapped FeS-graphene nanoribbons with improved cycling stability for lithium ion batteries

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Nano Research 2016年第10期9卷 2904-2911页

作者： Lei Li Caitian Gao Anton Kovalchuk Zhiwei Peng Gedeng Ruan Yang Yang huilong fei Qifeng Zhong Yilun Li James M. Tour Department of Chemistry Rice University 5100 Main Street Houston Texas 77005 USA School of Physical Science and Technology Lanzhou University Lanzhou 730000 China NanoCarbon Center Rice University 6100 Main Street Houston Texas 77005 USA State Key Laboratory of Bioelectronics School of Biological Science and Medical Engineering Southeast University Nanjing 210096 China Department of Materials Science and NanoEngineering Rice University 6100 Main Street Houston Texas 77005 USA

Sandwich structured graphene-wrapped FeS-graphene nanoribbons （G@FeS-GNIKs） were developed. In this composite, FeS nanoparticles were sandwiched between graphene and graphene nanoribbons. When used as anodes in lithium ion batteries （L1Bs）, the G@FeS-GNR composite demonstrated an outstanding electrochemical performance. This composite showed high reversible capacity, good rate performance, and enhanced cycling stability owing to the synergy between the electrically conductive graphene, graphene nanoribbons, and FeS. The design concept developed here opens up a new avenue for constructing anodes with improved electrochemical stability for LIBs.

关键词： lithium ion battery iron sulfide graphene nanoribbons graphene energy storage

Ultra-stable and High-rate Lithium Ion Batteries Based on Metal-organic Framework-derived ln2O3 Nanocrystals/Hierarchically Porous Nitrogen-doped Carbon Anode

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Energy & Environmental Materials 2020年第2期3卷 177-185页

作者： Hanjiao Xu Lei Wang Jiang Zhong Tao Wang Jinhui Cao Yaya Wang Xiuqi Li huilong fei Jian Zhu Xidong Duan State Key Laboratory for Chemo/Biosensing and Chemometrics College of Chemistry and Chemical EngineeringHunan Key Laboratory of TwoDimensional MaterialsHunan UniversityChangsha 410082China

Exploring electrode materials with attractive specific capacity and prominent cyclic durability is of the essence for promoting lithium ion batteries(LIBs).In2O3 has shown an extraordinary promise for LIBs with advantageous gravimetric capacity(theoretically 965 mA h g-1) and low working ***,In2O3 still suffers from the inherent weaknesses of metal oxides in practical application,especially low conductivity and incorrigible volume expansion upon the cycling ***,we demonstrate the architecture of metal-organic framework(MOF)-derived In2O3 nanocrystals/hierarchically porous nitrogen-doped carbon composite(In2O3/HPNC) for ultra-stable LIBs *** hierarchically porous structure(micro/meso/macro-pores) with nitrogen doping not only ensures exceptional mechanical strength and accommodates the volume expansion of In2O3 nanocrystals,but also offers electrons and lithium ions efficient interpenetrating pathways to migrate rapidly during charge/discharge ***,In2O3/HPNC exhibits excellent cyclic stability with a high specific capacity of 623 mA h g-1 over2000 cycles at 1000 mA g-1,corresponding to an ultra-low specific capacity decay of 0.017% per cycle(the best among the ln203-based anode for LIBs),and outstanding rate performance,suggesting a critical step toward achieving long-life and high-rate LIBs in practical devices.

关键词： hierarchically porous structure In203 nanocrystals metal-organic frameworks nitrogen-doping carbon ultra-stable lithium ion batteries

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The promises, challenges and pathways to room-temperature sodium-sulfur batteries

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National Science Review 2022年第3期9卷 144-168页

作者： Lei Wang Tao Wang Lele Peng Yiliu Wang Meng Zhang Jian Zhou Maoxin Chen Jinhui Cao huilong fei Xidong Duan Jian Zhu Xiangfeng Duan State Key Laboratory for Chemo Biosensing and Chemometricsand College of Chemistry and Chemical EngineeringHunan Key Laboratory of Two-Dimensional Materials Hunan University Department of Chemistry and Biochemistry University of CaliforniaLos Angeles

Room-temperature sodium-sulfur batteries(RT-Na-S batteries) are attractive for large-scale energy storage applications owing to their high storage capacity as well as the rich abundance and low cost of the ***, their practical application is hampered by severe challenges, such as low conductivity of sulfur and its reduced products, volume expansion, polysulfide shuttling effect and Na dendrite formation,which can lead to rapid capacity fading. The review discusses the Na-S-energy-storage chemistry,highlighting its promise, key challenges and potential strategies for large-scale energy storage ***, we review the electrochemical principles and the current technical challenges of RT-Na-S batteries, and discuss the strategies to address these obstacles. In particular, we give a comprehensive review of recent progresses in cathodes, anodes, electrolytes, separators and cell configurations, and provide a forward-looking perspective on strategies toward robust high-energy-density RT-Na-S batteries.

关键词： room-temperature sodium-sulfur batteries sulfur cathodes polysulfide shuttling effects Na dendrite formation electrocatalysis

Preparation of carbon-coated iron oxide nanoparticles dispersed on graphene sheets and applications as advanced anode materials for lithium-ion batteries

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Nano Research 2014年第4期7卷 502-510页

作者： huilong fei Zhiwei Peng Lei Li Yang Yang Wei Lu Errol L. G. Samuel Xiujun Fan James M. Tour Department of Chemistry Rice University 6100 Main Street Houston Texas 77005 USA Richard E. Smalley Institute for Nanoscale Science and Technology Rice University 6100 Main Street Houston Texas 77005 USA Department of Materials Science and NanoEngineering Rice University 6100 Main Street Houston Texas 77005 USA

We report a novel chemical vapor deposition （CVD） based strategy to synthesize carbon-coated Fe203 nanoparticles dispersed on graphene sheets （Fe2Og@C@G）. Graphene sheets with high surface area and aspect ratio are chosen as space restrictor to prevent the sintering and aggregation of nanoparticles during high temperature treatments （800 ℃）. In the resulting nanocomposite, each individual Fe2O3 nanoparticle （5 to 20 nm in diameter） is uniformly coated with a continuous and thin （two to five layers） graphitic carbon shell. Further, the core-shell nanoparticles are evenly distributed on graphene sheets. When used as anode materials for lithium ion batteries, the conductive-additive-free Fe2OB@C@G electrode shows outstanding Li＋ storage properties with large reversible specific capacity （864 mAh/g after 100 cycles）, excellent cyclic stability （120% retention after 100 cycles at 100 mA/g）, high Coulombic efficiency （-99%）, and good rate capability.

关键词： Fe2O3 nanoparticles carbon coating graphene chemical vapor deposition(CVD) anode lithium ion batteries