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Chinese Journal of Chemical Engineering 2021年第9期34卷 159-167页

作者： Chun Yao jiangwei chang Yiwang Ding chang Yu Jieshan Qiu State Key Laboratory of Fine Chemicals Liaoning Key Laboratory for Energy Materials and Chemical EngineeringSchool of Chemical EngineeringDalian University of TechnologyDalian 116024China

Carbon nanotubes(CNTs)have been far and wide employed as the counter electrodes(CEs)in dyesensitized solar cells because of their individual physical and chemical ***,the techniques available now,such as chemical vapor deposition,arc discharge and laser ablation for synthesizing CNTs,commonly suffer from rigorous operations and complicated steps,which make the process difficult to be ***,we present a simple and facile glutamic acid-assisted hydrothermal recrystallization strategy to construct bamboo-like CNTs(GHP-BC-x).Generally,the conventional organic dye3,4,9,10-perylene tetracarboxylic dianhydride(PTCDA)is used as a precursor and glutamic acid efficiently promotes the recrystallization of the perylene cores'planarπ-conjugated system in PTCDA under hydrothermal conditions and then self-assembles into one-dimensio nal nano rods with improved crystallization degree,finally resulting in the morphology of bamboo-like CNTs after *** applied as the counter electrodes,the GHP-BC-3 displays a remarkable power conversion efficiency of8.25%,benefiting from the superb electrical conductivity and mass transfer dynamics,superior to that of Pt CE(7.62%).

关键词： Hydrothermal recrystallization Bamboo-like carbon nanotubes Counter electrodes Electrocatalysis Triiodide reduction

N-doped carbon dots coupled NiFe-LDH hybrids for robust electrocatalytic alkaline water and seawater oxidation

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Nano Research 2022年第8期15卷 7063-7070页

作者： Peng Ding Haoqiang Song jiangwei chang Siyu Lu Green Catalysis Center and College of ChemistryZhengzhou UniversityZhengzhou 450000China

Electrolysis of seawater offers a highly promising and sustainable route to attain carbon-neutral hydrogen energy without demanding on high-purity water ***,it is severely limited by the undesirable chlorine oxidation reaction(ClOR)on the anode and the releasing toxic chlorine species,inducing anode corrosion and multiple pollutions to reduce the efficiency and sustainability of this *** effective way is to limit the overpotential of oxygen evolution reaction(OER)below 480 mV and thus suppress the ***,we demonstrate that nitrogen-doped carbon dots strongly coupled NiFe layered double hydroxide nanosheet arrays on Ni foam(N-CDs/NiFe-LDH/NF)can efficiently facilitate OER with an ultralow overpotential of 260 mV to deliver the geometric current density of 100 mA·cm^(−2)and a Tafel slope of as low as 43.4 mV·dec−1 in 1.0 M *** importantly,the N-CDs/NiFe-LDH/NF electrode at 100 mA·cm^(−2)shows overpotentials of 285 and 273 mV,respectively,by utilizing 1.0 M KOH with 0.5 M NaCl and 1.0 M KOH with 1.0 M NaCl as the simulated seawater,well avoid triggering ***,despite the complex environment of real seawater,N-CDs/NiFe-LDH/NF still effectively promotes alkaline seawater(1.0 M KOH+seawater)electrolysis with a lifetime longer than 50 and 20 h,respectively,in 1.0 M KOH and alkaline seawater *** investigation result reveals that M–N–C bonding generated between N-CDs and NiFe-LDH intrinsically optimizes the charge transfer efficiency,further promoting the OER kinetics.

关键词： N-doped carbon dots electrocatalysis oxygen evolution reaction(OER) seawater oxidation chlorine oxidation reaction(ClOR)

Fabrication of a nano-sized ZSM-5 zeolite with intercrystalline mesopores for conversion of methanol to gasoline

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Journal of Energy Chemistry 2017年第1期26卷 139-146页

作者： Tingjun Fu jiangwei chang Juan Shao Zhong Li Key Laboratory of Coal Science and Technology Ministry of Education and Shanxi ProvinceTaiyuan University of TechnologyTaiyuan 030024ShanxiChina

Carbon deposition during methanol to hydrocarbons leads to the quick deactivation of ZSM-5 catalyst and it is one of the major problems for this technology. Decreasing the crystal size or introducing mesopores into ZSM-5 zeolites can improve its diffusion property and decrease the coke formation. In this paper, nano-sized ZSM-5 zeolite with intercrystalline mesopores combining the mesoporous and nano sized structure was fabricated. For comparison, the mesoporous ZSM-5 and nano-sized ZSM-5 were also prepared. These catalyst samples were characterized by XRD, BET, NH3-TPD, TEM, Py-IR and TG techniques and used on the conversion of methanol to gasoline in a fixed-bed reactor at T=405 degrees C, WHSV =4.74 h(-1) and P=1.0 MPa. It was found that the external surface area of the nano-sized ZSM-5 zeolite with intercrystalline mesopores reached 104 m(2)/g, larger than that of mesoporous ZSM-5 (66 m(2)/g) and nano sized ZSM-5 (76 m(2)/g). Catalytic lifetime of the nano-sized ZSM-5 zeolite with intercrystalline mesopores was 93 h, which was only longer than that of mesoporous ZSM-5 (86 h), but shorter than that of nano sized ZSM-5 (104 h). Strong acidity promoted the coke formation and thus decreased the catalytic lifetime of the nano-sized ZSM-5 zeolite with intercrystalline mesopores though it presented large external surface that could improve the diffusion property. The special zeolite catalyst was further dealuminated to decrease the strong acidity. After this, its coke formation rate was slowed and catalytic lifetime was prolonged to 106 h because of the large external surface area and decreased weak acidity. This special structural zeolite is a potential catalyst for methanol to gasoline reaction. (C) 2016 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights reserved.

关键词： ZSM-5 Crystal size Mesopore Acidity Methanol to gasoline

Progress on the mechanisms of Ru-based electrocatalysts for the oxygen evolution reaction in acidic media

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Journal of Energy Chemistry 2023年第10期85卷 220-238,I0008页

作者： Yuanyuan Shi Han Wu jiangwei chang Zhiyong Tang Siyu Lu Green Catalysis Center and College of ChemistryZhengzhou UniversityZhengzhou 450001HenanChina CAS Key Laboratory of Nanosystem and Hierarchical Fabrication CAS Center for Excellence in NanoscienceNational Center for Nanoscience and TechnologyBeijing 100190China

Water electrolysis using proton-exchange membranes is one of the most promising technologies for carbon-neutral and sustainable energy ***,the overall efficiency of water splitting is limited by the oxygen evolution reaction(OER).Nevertheless,a trade-off between activity and stability exists for most electrocatalytic materials in strong acids and oxidizing media,and the development of efficient and stable catalytic materials has been an important focus of *** this view,gaining in-depth insights into the OER system,particularly the interactions between reaction intermediates and active sites,is significantly *** this end,this review introduces the fundamentals of the OER over Ru-based materials,including the conventional adsorbate evolution mechanism,lattice oxygen oxidation mechanism,and oxide path ***,the up-to-date progress of representative modifications for improving OER performance is further discussed with reference to specific mechanisms,such as tuning of geometric,electronic structures,incorporation of proton acceptors,and optimization of metal-oxygen ***,some valuable insights into the challenges and opportunities for OER electrocatalysts are provided with the aim to promote the development of next-generation catalysts with high activity and excellent stability.

关键词： Oxygen evolution reaction Ru-based electrocatalysts Acidic solutions Mechanism Proton-exchange membranes

Electrocatalytic water splitting:Mechanism and electrocatalyst design

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Nano Research 2023年第7期16卷 9142-9157页

作者： Han Wu Qiaoxian Huang Yuanyuan Shi jiangwei chang Siyu Lu Green Catalysis Center College of ChemistryZhengzhou UniversityZhengzhou 450001China

Hydrogen energy,a new type of clean and efficient energy,has assumed precedence in decarbonizing and building a sustainable carbon-neutral ***,hydrogen production from water splitting has seen considerable advancements owing to its advantages such as zero carbon emissions,safety,and high product *** overcome the large energy barrier and high cost of water splitting,numerous efficient electrocatalysts have been designed and ***,various difficulties in promoting the industrialization of electrocatalytic water splitting ***,as high-performance electrocatalysts that satisfy industrial requirements are urgently needed,a better understanding of water-splitting systems is *** this paper,the latest progress in water electrolysis is reviewed,and experimental evidence from in situ/operando spectroscopic surveys and computational analyses is summarized to present a mechanistic understanding of hydrogen and oxygen evolution ***,some promising strategies,including alloying,morphological engineering,interface construction,defect engineering,and strain engineering for designing and synthesizing electrocatalysts are *** believe that this review will provide a knowledge-guided design in fundamental science and further inspire technical engineering developments for constructing efficient electrocatalysts for water splitting.

关键词： water splitting mechanism operando spectroscopy design strategy

Intrinsic pentagon defect engineering in multiple spatial-scale carbon frameworks for efficient triiodide reduction

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Journal of Energy Chemistry 2024年第8期95卷 20-28,I0002页

作者： Siyi Hou Xuedan Song chang Yu jiangwei chang Yiwang Ding Yingbin Liu Xiubo Zhang Weizhe Liu Jieshan Qiu State Key Lab of Fine Chemicals Liaoning Key Lab for Energy Materials and Chemical EngineeringFrontier Science Center for Smart MaterialsSchool of Chemical EngineeringDalian University of TechnologyDalian 116024LiaoningChina Liaoning Key Lab for Energy Materials and Chemical Engineering Frontier Science Center for Smart MaterialsSchool of ChemistryDalian University of TechnologyDalian 116024LiaoningChina State Key Laboratory of Chemical Resource Engineering College of Chemical EngineeringBeijing University of Chemical TechnologyBeijing 100029China

Intrinsic topological defect engineering has been proven as a promising strategy to elevate the electrocatalytic activity of carbon ***,the controllable construction of high-density and specific topological defects in carbon frameworks to reveal the relationship between reactivity and defect structure remains a challenging ***,the intrinsic pentagon carbon sites that can favor electron overflow and enhance their binding affinity towards the intermediates of catalytic reaction are firstly presented by the work function and the p-band center *** experimentally verify this,the cage-opening reaction of fullerene is proposed and utilized for synthesizing carbon quantum dots with specific pentagon configuration(CQDs-P),subsequently utilizing CQDs-P to modulate the micro-scale defect density of three-dimensional reduced graphene oxide(rGO)viaπ-π*** multiple spatial-scale rGO-conjugated CQDs-P structure simultaneously possesses abundant pentagon and edge defects as catalytic active sites and long-range-orderedπelectron delocalization system as conductive *** defects-rich CQDs-P/rGO-4 all-carbon-based catalyst exhibits superb catalytic activity for triiodide reduction reaction with a high photoelectric conversion efficiency of 8.40%,superior to the Pt reference(7.97%).Theoretical calculations suggest that pentagon defects in the carbon frameworks can promote charge transfer and modulate the adsorption/dissociation behavior of the reaction intermediates,thus enhancing the electrocatalytic activity of the *** work confirms the role of intrinsic pentagon defects in catalytic reactions and provides a new insight into the synthesis of defects-rich carbon catalysts.

关键词： Defect engineering Pentagon carbon Carbon quantum dots Electrocatalytic activity Triiodide reduction

Design strategies towards transition metal single atom catalysts for the oxygen reduction reaction-A review

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Nano Research Energy 2023年第4期2卷 160-182页

作者： Yaojia Cheng Hao Wang Haoqiang Song Kan Zhang Geoffrey I.N.Waterhouse jiangwei chang Zhiyong Tang Siyu Lu Green Catalysis Center and College of ChemistryZhengzhou UniversityZhengzhou 450001China School of Materials Science and Engineering Nanjing University of Science and TechnologyNanjing 210094China School of Chemical Sciences The University of AucklandAuckland 1142New Zealand CAS Key Laboratory of Nanosystem and Hierarchical Fabrication National Center for Nanoscience and TechnologyBeijing 100190China

The electrochemical oxygen reduction reaction(ORR)is pivotal in energy conversion via a 4e-ORR pathway and green hydrogen peroxide production via 2e-ORR *** metal single atom catalysts(TM SACs)have attracted intense attention in recent years for ORR due to their high activity and near maximum metal atom *** future development of TM SACs for ORR requires improved understanding of reaction pathways,since currently the true origin of activity remains contentious owing to the lack of qualitative/quantitative information about active ***-guided design is imperative for the optimization of TM SACs performance in terms of activity and *** review focuses on the latest progress in the design of TM SACs for ORR,placing particular attention on efforts to elucidate reaction *** evidence based on in-situ/operando characterization measurements,along with theoretical predictions,are summarized to deepen understanding of the structure-performance relationships at both atomic and molecular ***,some perspectives are offered relating to the fundamental science needed for TM SACs to find practical application in energy storage and conversion *** hope this review will inspire the development of new synthetic routes towards high-performance ORR electrocatalysts for the energy sector.

关键词： oxygen reduction reaction 4/2e-pathway transition metals single-atom catalysts theoretical calculations in-situ/operando characterization measurements

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碳点的制备及电化学能源应用进展

高等学校化学学报 2023年第5期44卷 236-247页

作者：王斯阳敬稳常江伟卢思宇郑州大学化学学院绿色催化中心郑州450001

碳点是零维纳米碳材料的一种典型代表,由碳原子sp^(2)/sp^(3)杂化构成且尺寸通常小于10 nm.碳点独特的尺寸效应赋予其丰富的边缘活性位点和易于功能化调控等特性,在电催化、能源存储与转化等领域表现出广阔的应用前景.基于此,揭示碳点... 详细信息

碳点是零维纳米碳材料的一种典型代表,由碳原子sp^(2)/sp^(3)杂化构成且尺寸通常小于10 nm.碳点独特的尺寸效应赋予其丰富的边缘活性位点和易于功能化调控等特性,在电催化、能源存储与转化等领域表现出广阔的应用前景.基于此,揭示碳点的形成机制及阐明其结构与性能的基本规律,以指导碳点的合成并获得优异的催化性能具有重要意义.本文在介绍碳点制备及调控策略的基础上,结合理论研究分析了碳点类催化材料活性的来源,并着重评述了碳点在电化学领域的最新应用进展,探讨了功能碳点材料未来发展的机遇与挑战.

关键词：碳点电化学能源存储与转化理论计算

碳分子筛的优化设计及其I3^−还原性能研究

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化工学报 2020年第6期71卷 2696-2704页

作者：姚春黄龙龙常江伟丁一旺于畅邱介山大连理工大学化工学院辽宁省能源材料化工重点实验室精细化工国家重点实验室辽宁大连116024 北京化工大学化学工程学院北京100029

研究对比了商业化碳分子筛(CMS)、多壁碳纳米管、活性炭和还原氧化石墨烯四种碳材料的I3−还原性能。采用场发射扫描电镜、高倍率透射电镜、X射线衍射等技术手段表征了材料的微观结构特征,结合循环伏安(CV)和光电转换测试(I-V)结果,解耦... 详细信息

研究对比了商业化碳分子筛(CMS)、多壁碳纳米管、活性炭和还原氧化石墨烯四种碳材料的I3−还原性能。采用场发射扫描电镜、高倍率透射电镜、X射线衍射等技术手段表征了材料的微观结构特征,结合循环伏安(CV)和光电转换测试(I-V)结果,解耦了材料的构效关系。结果发现,以CMS为对电极组装的DSSCs的光电转换效率最高,达7.46%。在此基础上,研究考察了高温退火处理对CMS的微观结构、性质和性能的影响,揭示了影响I3^−还原性能的关键因素。结果表明,800℃处理的样品CMS800光电转换效率高达8.56%,明显优于贵金属Pt对电极,同时表现出优于Pt的电化学稳定性。

关键词：染料敏化太阳能电池碳分子筛光电转换效率催化活性 I3^−还原

Carbon dots-derived carbon nanoflowers decorated with cobalt single atoms and nanoparticles as efficient electrocatalysts for oxygen reduction

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Chinese Journal of Catalysis 2022年第9期43卷 2443-2452页

作者： Yaojia Cheng Haoqiang Song Jingkun Yu jiangwei chang Geoffrey I.N.Waterhouse Zhiyong Tang Bai Yang Siyu Lu Green Catalysis Center and College of Chemistry Zhengzhou UniversityZhengzhou 450000HenanChina College of Chemistry and Chemical Engineering Jishou UniversityJishou 416000HunanChina School of Chemical Sciences The University of AucklandAuckland 1142New Zealand CAS Key Laboratory of Nanosystem and Hierarchical Fabrication National Center for Nanoscience and TechnologyBeijing 100190China State Key Laboratory of Supramolecular Structure and Materials College of Chemistry Jilin UniversityChangchun 130012JilinChina

The sluggish kinetics of oxygen reduction reaction(ORR)hinders the commercialization of Zn‐air batteries(ZABs).Manipulating the electronic structure of electrocatalysts to optimize the adsorption energy of oxygen‐containing intermediates during the 4e–ORR offers a practical route toward improving ORR ***,we designed a novel ORR electrocatalyst containing Co single atoms and nanoparticles supported by carbon dots‐derived carbon nanoflowers(Co SAs/NPs CNF).Co SAs/NPs CNF possessed a very high ORR activity(E_(1/2) of the Co SAs/NPs CNF catalyst is 0.83 V(***)),and outstanding catalytic performance and stability when used as the air‐electrode catalyst in rechargeable ZABs(152.32 mW cm^(-2),1000.58 mWh gZn^(–1),and over 1300 cycles at a current density of 5 mA cm^(-2)).The Co SAs and Co NPs cooperated to improve electron and proton transfer processes during *** calculations revealed that the presence of adjacent Co NPs optimized the electronic structure of the isolated Co‐N_(4) sites,significantly lowering the energy barriers for the rate‐determining step in ORR(adsorption of*OOH)and thereby delivering outstanding ORR *** work reveals that the combination of supported single‐atom sites and metal nanoparticles can be highly beneficial for ORR electrocatalysis,outperforming catalysts containing only Co SAs or Co NPs.

关键词： Carbon dots Co single atom Co nanoparticle Oxygen reduction reaction Zn-air battery

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