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Defect Engineering on Carbon‑Based Catalysts for Electrocatalytic CO2 Reduction

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Nano-Micro Letters 2021年第1期13卷 56-78页

作者： Dongping Xue huicong xia Wenfu Yan Jianan Zhang Shichun Mu College of Materials Science and Engineering Zhengzhou UniversityZhengzhou 450001People’s Republic of China State Key Laboratory of Inorganic Synthesis and Preparative Chemistry and College of ChemistryJilin University2699 Qianjin StreetChangchun 130012People’s Republic of China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070People’s Republic of China

Electrocatalytic carbon dioxide(CO2)reduction(ECR)has become one of the main methods to close the broken carbon cycle and temporarily store renewable energy,but there are still some problems such as poor stability,low activity,and *** the most promising strategy to improve ECR activity is to develop electrocatalysts with low cost,high activity,and long-term ***,defective carbon-based nanomaterials have attracted extensive attention due to the unbalanced electron distribution and electronic structural distortion caused by the defects on the carbon ***,the present review mainly summarizes the latest research progress of the construction of the diverse types of defects(intrinsic carbon defects,heteroatom doping defects,metal atomic sites,and edges detects)for carbon materials in ECR,and unveil the structure-activity relationship and its catalytic *** current challenges and opportunities faced by high-performance carbon materials in ECR are discussed,as well as possible future *** can be believed that this review can provide some inspiration for the future of development of high-performance ECR catalysts.

关键词： Electrocatalytic CO2 reduction Carbon-based nanomaterials Intrinsic defects Heteroatom doping defects Metal atomic sites

Mechanism of interfacial effects in sodium-ion storage devices

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Nano Research 2024年第3期17卷 1313-1326页

作者： Yifan Wei Lingxing Zan huicong xia Wenfu Yan Jia-Nan Zhang College of Materials Science and Engineering Zhengzhou UniversityZhengzhou 450001China Key Laboratory of Advanced Energy Catalytic and Functional Material Preparation of Zhengzhou City Zhengzhou 450001China Key Laboratory of Chemical Reaction Engineering of Shaanxi Province College of Chemistry&Chemical EngineeringYan’an UniversityYan’an 716000China State Key Laboratory of Inorganic Synthesis and Preparative Chemistry and College of Chemistry Jilin UniversityChangchun 130012China

Rechargeable sodium-ion batteries(SIBs)are considered as the next-generation secondary *** performance of SIB is determined by the behavior of its electrode surface and the electrode–electrolyte interface during charging and ***,the characteristics of these surfaces and interfaces should be analyzed to realize large-scale energy storage systems with high energy density and long-cycle *** various studies have investigated the properties of electrode materials,few studies have focused on the construction of stable and efficient SIB interfaces,and even fewer have explored the mechanisms of interfacial effects;however,the strategies of regulating interfacial effects are yet to be completely ***,the results obtained thus far are insufficient to draw systematic *** present study reviews the literature on the mechanism of interfacial effects in Na+storage *** interfaces in a sodium-ion storage device include a heterogeneous interface between electrode materials,a solid electrolyte interphase,and a cathode electrolyte *** interfacial effects during the intercalation,transformation,and alloy reactions and the resulting overall battery performance were theoretically *** this review,we aim to provide a theoretical basis for optimizing the structures of electrode surface and electrode–electrolyte interface to optimize the performance of *** addition,the challenges of investigating interfacial effects and several possible helpful methods and opportunities for studying the mechanisms of interfacial effects in SIBs will be presented.

关键词： sodium-ion storage interfacial effects solid electrolyte interphase cathode electrolyte interphase

Atomic Level Dispersed Metal–Nitrogen–Carbon Catalyst toward Oxygen Reduction Reaction: Synthesis Strategies and Chemical Environmental Regulation

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Energy & Environmental Materials 2021年第1期4卷 5-18页

作者： Hengbo Yin huicong xia Shuyan Zhao Kexie Li Jianan Zhang Shichun Mu College of Materials Science and Engineering Zhengzhou UniversityZhengzhou 450001China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China

For development and application of proton exchange membrane fuel cell(PEMFC) energy transformation technology, the cost performance must be elevated for the catalyst. At present, compared with noble metal-based catalysts, such as Pt-based catalysts, atomically dispersed metal–nitrogen–carbon(M–N–C) catalysts are popularity and show great potential in maximizing active site density, high atom utilization and high activity,making them the first choice to replace Pt-based catalysts. In the preparation of atomically dispersed metal–nitrogen–carbon catalyst, it is difficult to ensure that all active sites are uniformly dispersed, and the structure system of the active sites is not optimal. Based on this, we focus on various approaches for preparing M–N–C catalysts that are conducive to atomic dispersion, and the influence of the chemical environmental regulation of atoms on the catalytic sites in different catalysts. Therefore, we discuss the chemical environmental regulation of the catalytic sites by bimetals, atom clusters, and heteroatoms(B, S, and P). The active sites of M–N–C catalysts are explored in depth from the synthesis and characterization, reaction mechanisms, and density functional theory(DFT)calculations. Finally, the existing problems and development prospects of the current atomic dispersion M–N–C catalyst are proposed in detail.

关键词： atomic-level catalyst chemical environmental effects metal-nitrogen-carbon oxygen reduction reaction synthesis strategy

2D MOF Nanoflake-Assembled Spherical Microstructures for Enhanced Supercapacitor and Electrocatalysis Performances

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Nano-Micro Letters 2017年第4期9卷 62-72页

作者： huicong xia Jianan Zhang Zhao Yang Shiyu Guo Shihui Guo Qun Xu College of Materials Science and Engineering Zhengzhou University Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education) Nankai University State Key Laboratory of Inorganic Synthesis and Preparative Chemistry Jilin University

Metal–organic frameworks(MOFs) are of great interest as potential electrochemically active ***, few studies have been conducted into understanding whether control of the shape and components of MOFs can optimize their electrochemical performances due to the rational realization of their shapes. Component control of MOFs remains a significant challenge. Herein, we demonstrate a solvothermal method to realize nanostructure engineering of 2D nanoflake MOFs. The hollow structures withNi/Co-and Ni-MOF(denoted as Ni/Co-MOF nanoflakes and Ni-MOF nanoflakes) were assembled for their electrochemical performance optimizations in supercapacitors and in the oxygen reduction reaction(ORR). As a result, the Ni/CoMOF nanoflakes exhibited remarkably enhanced performance with a specific capacitance of 530.4 F g^(-1)at 0.5 A g^(-1)in1 M LiO H aqueous solution, much higher than that of NiMOF(306.8 F g^(-1)) and ZIF-67(168.3 F g^(-1)), a good rate capability, and a robust cycling performance with no capacity fading after 2000 cycles. Ni/Co-MOF nanoflakes also showed improved electrocatalytic performance for the ORR compared to Ni-MOF and ZIF-67. The present work highlights the significant role of tuning 2D nanoflake ensembles of Ni/Co-MOF in accelerating electron and charge transportation for optimizing energy storage and conversion devices.

关键词： Metal–organic frameworks Nanoflakes Spherical microstructure Supercapacitor Oxygen reduction reaction

Fabrication of Fe-doped Co-MOF with mesoporous structure for the optimization of supercapacitor performances

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Chinese Chemical Letters 2018年第6期29卷 834-836页

作者： Huanan Yu huicong xia Jianan Zhang Jing He Shiyu Guo Qun Xu College of Materials Science and Engineering Zhengzhou University Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education) Nankai University

The synergy effect between different components has attracted widespread attentions because of improved activity, selectivity and stability than single component. In this paper, we fabricated mesoporous hybrid dual-metal Co and Fe containing metallic organic framework（Co/Fe-MOF）, Fe-MOF,and Co-MOF in the ionic liquid（IL）/supercritical CO2（SC）/surfactant emulsion system, and then studied the electrochemical properties of the three MOFs systematically. Experiment results indicate that, by taking advantages of coexistence of double metal, hybrid bi-metal Co/Fe-MOF exhibits the highest specific capacitance and the best cycling stability, with specific capacitance to 319.5 F/g at 1 A/g, 1.4 and 4 times for single Co-MOF and Fe-MOF, respectively.

关键词： Metallic organic framework Mesoporous structure Synergistic effect Hybrid dual-metal Supercapacitor

Atomically Dispersed Fe-N_(4) Sites and Fe_(3)C Particles Catalyzing Polysulfides Conversion in Li-S Batteries

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Chemical Research in Chinese Universities 2022年第5期38卷 1232-1238页

作者： CHEN Weijie xia huicong GUO Kai JIN Wangzhe DU Yu YAN Wenfu QU Gan ZHANG Jianan College of Materials Science and Engineering Zhengzhou UniversityZhengzhou 450001P.R.China State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of ChemistryJilin UniversityChangchun 130012P.R.China

Lithium-sulfur(Li-S)batteries have been puzzled by the“shuttle effect”.In the recent years,catalytic materials present a huge potential for solving this ***,the exploitation for catalytic activity was still challenging in Li-S *** this article,we put forward a single atom catalyst(SAC)of FeN_(4) coupled with Fe_(3)C on the N-doped carbon(FeN_(4)/Fe_(3)C@NC)by one-step pyrolysis *** FeN_(4) and Fe_(3)C synergistically catalyze the polysulfides conversion when the N-doped carbon provides the high conductive three-dimensional skeleton in Li-S *** a result,the FeN_(4)/Fe_(3)C@NC shows a specific capacity of 1100 mA·h/g at 0.2 C(1 C=1675 mA/g).In addition,the FeN_(4)/Fe_(3)C@NC maintains 99.01%of the pristine specific capacity after 100 cycles at 0.5 C,indicating the improved electrochemical performance in Li-S *** work sheds new lights on the design of engineering catalysts for developing high-performance Li-S batteries.

关键词： FeN_(4) Fe_(3)C Li-S battery Shuttle effect

Work-function effect of Ti_(3)C_(2)/Fe-N-C inducing solid electrolyte interphase evolution for ultra-stable sodium storage

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Nano Research 2024年第8期17卷 7163-7173页

作者： huicong xia Lingxing Zan Hongliang Dong Yifan Wei Yue Yu Jinfu Shu Jia-Nan Zhang Chong-Xin Shan Key Laboratory of Advanced Energy Catalytic and Functional Material Preparation of Zhengzhou College of Materials Science and EngineeringZhengzhou UniversityZhengzhou 450001China Key Laboratory of Materials Physics of Ministry of Education School of Physics and MicroelectronicsZhengzhou UniversityZhengzhou 450001China Key Laboratory of Chemical Reaction Engineering of Shaanxi Province College of Chemistry and Chemical EngineeringYan’an UniversityYan’an 716000China Center for High Pressure Science and Technology Advanced Research PudongShanghai 201203China Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education) Nankai UniversityTianjin 300071China

In the quest to enhance the efficiency of sodium-ion batteries,the dynamics of solid electrolyte interphase(SEI)formation are of paramount *** SEI layer’s integrity is integral to the charge–discharge efficiency and the overall longevity of the ***,a novel two-dimensional Ti_(3)C_(2) fragments enmeshed on iron-nitrogen-carbon(Fe-N-C)nanosheets(Ti_(3)C_(2)/Fe-NC)has been *** electrode features a matrix which has been shown to expedite SEI layer formation through the facilitation of selective anion adsorption,thus augmenting battery *** functional theory calculation reveals that the SEI evolution energy of NaPF6 at the Ti_(3)C_(2)/Fe-N-C interface is 0.81 eV,significantly lower than the Ti_(3)C_(2)(1.23 eV).This process is driven by the electron transportation from Ti_(3)C_(2) to Fe-N-C substrate,facilitated by their work-function difference,leading to the formation of ferromagnetic Fe species,which possesses Fe 3d d_(xz)d_(z)2 orbitals and undergoes hybridization with theπandσorbitals of NaF,creating a key intermediate during *** process diminishes the antibonding energy and attenuates the orbital interaction with NaF,thus reducing the activation energy and improving the SEI formation reaction ***,it leads to the creation of multi-interface SEI characterized by high-throughput ion transport and an efficient reaction network.

关键词： Ti_(3)C_(2)/Fe-N-C heterostructure work-function electron interaction solid electrolyte interphase sodium storage

Rational confinement engineering of MOF-derived carbonbased electrocatalysts toward CO_(2)reduction and O_(2)reduction reactions

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InfoMat 2022年第3期4卷 34-63页

作者： xiaoyu Zhang Dongping Xue Su Jiang huicong xia Yanlin Yang Wenfu Yan Jinsong Hu Jianan Zhang College of Materials Science and Engineering Zhengzhou UniversityZhengzhouP.R.China Academic Publishing Center Henan Polytechnic UniversityJiaozuoP.R.China State Key Laboratory of Inorganic Synthesis and Preparative Chemistry and College of ChemistryJilin UniversityChangchunP.R.China Beijing National Laboratory for Molecular Sciences(BNLMS) Institute of ChemistryChinese Academy of SciencesBeijingP.R.China

The goal of global carbon peak and neutrality gives an impetus to the utilization of clean energy(e.g.,fuel cell)and carbon dioxide(CO_(2))at a large scale,where the oxygen reduction reaction(ORR)and CO_(2)reduction reaction(CO_(2)RR)are the key reactions via the sustainable system,*** a main precursor for fabricating affordable carbon-based electrocatalysts with uniformly dispersed active centers and tailorable performances for ORR and CO_(2)RR,metal organic frameworks(MOFs)have captured a surge of interest in recent *** the facilitated development of MOF-derived carbon-based electrocatalysts by many investigations,it is still plagued by high overpotential and unsatisfied life span,which are greatly determined by the efficient and alterable confinement effect on synthesis and *** this review,firstly,the confined synthetic strategies(doping engineering,defect engineering,geometric engineering,etc.)of MOF-derived carbon-based electrocatalysts with multi-sized active centers(atom,atomic clusters and nanoparticles(NPs))are systematically summarized;secondly,the confinement effect on the interaction of ORR and CO_(2)RR intermediates,as well as the catalytic durability and activity,was discussed from chemical and physical *** the end,the review discusses the remaining challenges and emerging research topics in the future,including support upgradation and catalyst innovation,high selectivity and effective confinement synthesis,in situ and operando characterization techniques,theoretical investigation,and artificial intelligence(AI)*** new understanding and insights into these aspects will guide the rational confinement concept of MOF-derived carbon-based electrocatalysts for ORR and CO_(2)RR with optimized performances in terms of confinement engineering and are believed to be helpful for filling the existing gaps between scientific communities and practical use.

关键词： carbon-based materials CO_(2)reduction reaction confinement effect electrocatalyst metal organic framework oxygen reduction reaction

3D MoS_(2) foam integrated with carbon paper as binder-free anode for high performance sodium-ion batteries

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Journal of Energy Chemistry 2022年第2期31卷 26-33页

作者： Fangying Zheng Zeyu Wei huicong xia Yunchuan Tu xiangyu Meng Kaixin Zhu Jiao Zhao Yimin Zhu Jianan Zhang Yan Yang Dehui Deng Institute of Environmental Remediation Dalian Maritime UniversityDalian 116026LiaoningChina State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina College of Materials Science and Engineering Zhengzhou UniversityZhengzhou 450001HenanChina Zhang Dayu School of Chemistry Dalian University of TechnologyDalian 116024LiaoningChina

Molybdenum sulfide(MoS_(2))with well-designed porous structure has the potential to be great electrode materials in sodium-ion batteries due to its high theoretical capacity and abundant resource,however,hindered by its intrinsic low conductivity and ***,MoS_(2) with 3 D macroporous foam structure and high conductivity was obtained through SiO_(2) templates and integrated with carbon paper(3 D FMoS_(2)/CP).It has showed superior specific capacity(225 m A h g^(-1),0.4–3 V)and cycling stability(1000 cycles)at high rate(2000 m A g^(-1)),with a low decay rate(0.033%per cycle)in sodium-ion *** excellent electrochemical performance may originate from its unique integrated structure:3 D MoS_(2) macropores providing high surface area and abundant transfer channels while carbon paper enhancing the conductivity of MoS_(2) and avoiding unnecessary side reactions brought by binder addition.

关键词： 3D MoS_(2)foam Carbon paper Binder-free electrode High performance Sodium-ion batteries