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Journal of Energy Chemistry 2024年第8期95卷 540-553,I0012页

作者： Yihan Lin Liheng Li Longjie Tan Yongliang Li Xiangzhong Ren Peixin Zhang chuanxin he Lingna Sun College of Chemistry and Environmental Engineering Shenzhen UniversityShenzhen 518060GuangdongChina

Although lithium-sulfur batteries(LSBs)exhibit high theoretical energy density,their practical application is hindered by poor conductivity of the sulfur cathode,the shuttle effect,and the irreversible deposition of Li_(2)*** address these issues,a novel composite,using electrospinning technology,consisting of Fe_(3)Se_(4)and porous nitrogen-doped carbon nanofibers was designed for the interlayer of *** porous carbon nanofiber structure facilitates the transport of ions and electrons,while the Fe_(3)Se_(4)material adsorbs lithium polysulfides(LiPSs)and accelerates its catalytic conversion ***,the Fe_(3)Se_(4)material interacts with soluble LiPSs to generate a new polysulfide intermediate,Li_(x)FeS_(y)complex,which changes the electrochemical reaction pathway and facilitates the three-dimensional deposition of Li_(2)S,enhancing the reversibility of *** designed LSB demonstrates a high specific capacity of1529.6 mA h g^(-1)in the first cycle at 0.2 *** rate performance is also excellent,maintaining an ultra-high specific capacity of 779.7 mA h g^(-1)at a high rate of 8 *** investigation explores the mechanism of the interaction between the interlayer and LiPSs,and provides a new strategy to regulate the reaction kinetics and Li_(2)S deposition in LSBs.

关键词： Lithium-sulfur batteries Polysulfide intermediates Li_(2)S electrodeposition Interlayers Electrostatic spinning Adsorption Catalysis

Building Fe atom–cluster composite sites using a site occupation strategy to boost electrochemical oxygen reduction

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Carbon Energy 2024年第3期6卷 276-286页

作者： Tingyi Zhou Yi Guan Changjie he Lei Zhang Xueliang Sun Zhongxin Song Qianling Zhang chuanxin he Xiantao Jiang Zhaoyan Luo Wei Xing Xiangzhong Ren College of Chemistry and Environmental Engineering Shenzhen UniversityShenzhenGuangdongChina Department of Mechanical and Materials Engineering University of Western OntarioLondonOntarioCanada State Key Laboratory of Electroanalytical Chemistry Jilin Province Key Laboratory of Low Carbon Chemical PowerChangchun Institute of Applied ChemistryChinese Academy of SciencesJilinChangchunChina

The high-temperature pyrolysis process for preparing M–N–C single-atom catalyst usually results in high heterogeneity in product structure concurrently contains multiscale metal phases from single atoms(SAs),atomic clusters to ***,understanding the interactions among these components,especially the synergistic effects between single atomic sites and cluster sites,is crucial for improving the oxygen reduction reaction(ORR)activity of M–N–C ***,herein,we constructed a model catalyst composed of both atomically dispersed FeN4 SA sites and adjacent Fe clusters through a site occupation *** found that the Fe clusters can optimize the adsorption strength of oxygen reduction intermediates on FeN4 SA sites by introducing electron-withdrawing–OH ligands and decreasing the d-band center of the Fe *** as-developed catalyst exhibits encouraging ORR activity with halfwave potentials(E1/2)of 0.831 and 0.905 V in acidic and alkaline media,***,the catalyst also represents excellent durability exceeding that of Fe–N–C SA *** practical application of Fe(Cd)–CNx catalyst is further validated by its superior activity and stability in a metalair battery *** work exhibits the great potential of synergistic effects between multiphase metal species for improvements of singleatom site catalysts.

关键词： d-band center metal clusters oxygen reduction reaction single-atom catalyst site occupations strategy

Electronic structure and geometric construction modulation of carbon-based single/dual atom catalysts for electrocatalysis

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Energy Reviews 2024年第3期3卷 76-91页

作者： Shaolong Zhang Jing Huang Li Ma Dong Zhai Bin Wei hengpan Yang chuanxin he College of Chemistry and Environmental Engineering Shenzhen UniversityShenzhen518060PR China Pharmaceutical College Guangxi Medical UniversityNanning530021PR China Key Laboratory of New Electric Functional Materials of Guangxi Colleges and Universities Nanning Normal UniversityNanning530023PR China Institute of Molecular Sciences and Engineering Institute of Frontier and Interdisciplinary ScienceShandong UniversityQingdao266237PR China School of Materials Sun Yat-sen UniversityShenzhen518107PR China

Both carbon-based single atom catalysts(SACs)and dual atom catalysts(DACs)have garnered significant attention in the field of electrochemical reactions because of the impressive attributes,including exceptional catalytic activity,selectivity,and *** ability to modulate the electronic structure and geometric construction of active sites within SACs/DACs is paramount for unleashing their complete potential,which in turn can ultimately dictate catalytic behavior with unprecedented *** this review,the recent major developments of the regulation strategies for modulating electronic structure and geometric construction of carbon-based SACs/DACs are *** the SACs,the recently reported modulation methods are categorized into four strategies,including adjusting the density of single atoms,defect engineering,confinement effect and strain *** for the DACs,the five methods contain bonded dual-atom adjustment,non-bonded and bridged dual-atom adjustment,metal and nonmetal dual-atom adjustment,bilayer dual-atom adjustment and homogeneous dual-atom *** recently developed synthetic strategies are comprehensively summarized,especially their electronic structure and geometric configuration are discussed in detail,the different catalytic applications of electrochemical reactions,and their unique catalytic mechanism are ***,the challenges and prospects of SACs/DACs for tailoring their electronic structures and geometric arrangements are further discussed.

关键词： Electronic structure Geometric construction Single atom catalysts Dual atom catalysts Modulation

Constructing hierarchical arrays with core-shell metal oxides@metal coordination polymers for efficient and stable overall water splitting

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Nano Research 2024年第6期17卷 4882-4888页

作者： Shuai Qi Jinlian Liao Kunzhong Chen Senkai Li Jinwen Zhao Tianchi Huang Na Meng hengpan Yang Qi Hu chuanxin he College of Chemistry and Environmental Engineering Shenzhen UniversityShenzhen 518060China

Developing non-precious metal-based bifunctional electrocatalysts capable for both hydrogen evolution reaction(heR)and oxygen evolution reaction(OER)is essential to achieve efficient water electrolysis for mass hydrogen production,however it remains ***,we report the synthesis of hierarchical nanorod arrays comprising core-shell structured P-doped NiMoO4@NiFe-coordination polymer(denoted as P-NiMoO4@NiFeCP)as bifunctional electrocatalysts for water ***,we systematically investigate the influence of NiFeCP shell thickness on electrocatalytic activity,manifesting the presence of strong interfacial synergetic effect between P-NiMoO4 and NiFeCP for boosting both the heR and *** advantageous hierarchical architectures and unique core-shell structures,optimized P-NiMoO_(4)@NiFeCP-7.3(7.3 is the shell thickness in nm)requires overpotentials of merely 256 and 297 mV to yield a current density of 1000 mA·cm^(−2)for the heR and OER in 1 M KOH,*** importantly,it can serve as a bifunctional electrocatalyst for efficient and sustainable overall water electrolysis,delivering large current densities of 500 and 1000 mA·cm^(−2)at low cell voltages of 1.804 and 1.865 V,along with high stability of over 500 h at 1000 mA·cm−2,demonstrating the great potential of this electrocatalyst towards practical applications.

关键词： hydrogen evolution reaction oxygen evolution reaction overall water splitting non-precious metal-based electrocatalysts core-shell structures

Boosting Electrochemical Urea Synthesis via Constructing Ordered Pd–Zn Active Pair

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Nano-Micro Letters 2024年第11期16卷 529-540页

作者： Weiliang Zhou Chao Feng Xuan Li Xingxing Jiang Lingyan Jing Shuai Qi Qihua Huo Miaoyuan Lv Xinbao Chen Tianchi Huang Jingwen Zhao Na Meng hengpan Yang Qi Hu chuanxin he College of Chemistry and Environmental Engineering Shenzhen UniversityShenzhen 518060GuangdongPeople’s Republic of China School of Chemistry and Chemical Engineering/State Key Laboratory Incubation Base for Green Processing of Chemical Engineering Shihezi UniversityShihezi 832003XinjiangPeople’s Republic of China

Electrochemical co-reduction of nitrate(NO_(3)^(-))and carbon dioxide(CO_(2))has been widely regarded as a promising route to produce urea under ambient conditions,however the yield rate of urea has remained ***,we report an atomically ordered intermetallic pallium-zinc(PdZn)electrocatalyst comprising a high density of PdZn pairs for boosting urea *** is found that Pd and Zn are responsible for the adsorption and activation of NO_(3)^(-)and CO_(2),respectively,and thus the co-adsorption and co-activation NO_(3)^(-)and CO_(2) are achieved in ordered PdZn *** importantly,the ordered and well-defined PdZn pairs provide a dual-site geometric structure conducive to the key C-N coupling with a low kinetical barrier,as demonstrated on both operando measurements and theoretical ***,the PdZn electrocatalyst displays excellent performance for the co-reduction to generate urea with a maximum urea Faradaic efficiency of 62.78%and a urea yield rate of 1274.42μg mg^(-1) h^(-1),and the latter is 1.5-fold larger than disordered pairs in PdZn *** work paves new pathways to boost urea electrosynthesis via constructing ordered dual-metal pairs.

关键词： Electrochemical C-N coupling Urea electrosynthesis Intermetallic compounds Geometric structures Active pairs

充分稳定和暴露的铜基异质结实现CO_(2)高效电还原制乙醇

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Chinese Journal of Catalysis 2024年第3期58卷 216-225页

作者：蒋兴星赵雨昕孔艳孙建桔冯上照胡琪杨恒攀何传新深圳大学化学与环境工程学院广东深圳518060

二氧化碳(CO_(2))虽然被视为破坏生态环境的温室气体,但也是储量最丰富的碳资源,对其进行转化和利用将对社会环境和能源结构产生深远影响.电化学还原CO_(2)(CO_(2)RR)不仅转化效率高,而且成本较低,有望实现规模化生产.在众多催化剂中,... 详细信息

二氧化碳(CO_(2))虽然被视为破坏生态环境的温室气体,但也是储量最丰富的碳资源,对其进行转化和利用将对社会环境和能源结构产生深远影响.电化学还原CO_(2)(CO_(2)RR)不仅转化效率高,而且成本较低,有望实现规模化生产.在众多催化剂中,廉价易得的铜基催化剂被认为是电化学催化还原CO_(2)生成高附加值产物的理想催化剂之一,其中铜氧化物的存在是CO_(2)RR生成高附加值产物的关键.然而,CO_(2)RR过程是在负电位下进行的,当施加电位低于‒0.1 VRhe时,铜氧化物很容易被还原为金属态铜.因此,催化剂稳定氧化态铜的能力在保持连续、高效和稳定的CO_(2)RR产多碳产物性能中至关重要.本文将简单的O_(2)等离子体处理技术与静电纺丝技术相结合,合成了多孔碳纳米纤维负载的Cu/Cu_(x)O异质结催化剂,并考察了其催化CO_(2)RR的性能.在静电纺丝过程中,Cu-ZIF-8前驱体的加入使得热处理后的原丝纤维中形成了丰富的网络贯穿多孔结构,该结构有效地实现了铜纳米颗粒的均匀分散;随后,通过O_(2)等离子体处理技术,在碳纳米纤维中构建了大量的开放介孔,为CO_(2)的吸附和反应提供了有利环境,并使Cu/Cu_(x)O异质结位点暴露于反应界面.电化学性能测试结果表明,在400 mA cm^(‒2)电流密度下,独特的Cu/Cu_(x)O异质结活性位点电催化还原CO_(2)生成乙醇的法拉第效率可达70.7%,该性能优于未经O_(2)等离子体处理的多孔铜纳米纤维.此外,高暴露的Cu/Cu_(x)O异质结活性位点显著地增加实际参与反应的活性位点数量,经计算Cu/Cu_(x)O异质结CO_(2)RR产乙醇的质量活性高达8.4 A mg^(‒1),是目前报道生产乙醇的较高质量活性.多孔碳纳米纤维衬底不仅具有协同电子输运能力,而且在CO_(2)RR测试中施加的负电压有助于维持Cu/Cu_(x)O异质结构的稳定性,使其在高电流密度下能够保持长时间的催化稳定性.此外,本文利用原位拉曼光谱和红外光谱、有限元模拟及密度泛函理论计算等方法深入研究了Cu/Cu_(x)O异质结的催化机理.原位拉曼光谱和红外光谱表征结果证实了在CO_(2)RR过程中Cu_(x)O的动态稳定状态以及关键信号*CO和C‒C键的存在;理论计算表明,Cu/Cu_(x)O异质结的存在促进了关键中间体*CO的溢流,降低了C‒C耦合过程的反应能垒,从而提高了还原产物乙醇的产率.综上,本文成功地在多孔铜纳米纤维中引入氧化物物种,并优化了纤维孔结构.其表现出了较好的电催化还原CO_(2)性能,可高选择性生成乙醇,其独特的多孔碳纤维结构充分暴露了活性位点,实现了较高的质量活性.本文所采用的催化剂组分和微观结构的调控策略为提升电催化中催化剂稳定性和催化活性提供了有益的借鉴.

关键词：二氧化碳电还原 Cu/Cu_(x)O异质结开口孔结构质量活性乙醇

Bimetallic two-dimensional materials for electrocatalytic oxygen evolution

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Chinese Chemical Letters 2022年第8期33卷 3657-3671页

作者： Xiaojie Li Qi Hu hengpan Yang Tao Ma Xiaoyan Chai chuanxin he College of Chemistry and Environmental Engineering Shenzhen UniversityShenzhen 518060China

Electrocatalytic oxygen evolution reaction(OER)is one of the important half reactions of electrocatalytic water ***,the slow kinetic process involving four-electron transfer severely limits its reaction efficiency,which in turn limits the overall electrocatalytic hydrolysis *** order to improve the activity of the electrocatalytic OER,researchers mainly update the catalyst from three aspects,that is,increase the conductivity of the electrocatalyst,and the quantity and quality of active ***(2 D)engineering can effectively reduce the resistance of the materials and greatly increase the number of electrochemically active sites,while heterometal doping,or the bimetal strategy,can improve the quality of active sites via changing the electronic structure of the ***,the combination of the two can enhance the activity of electrocatalytic OER in all three aspects:conductivity,number and quality of active ***,there is currently no review on this ***,in this review,we summarize the application of bimetallic 2 D materials in electrocatalytic OER from four aspects:the structure,synthesis strategy,catalytic efficiency,and reaction mechanism.

关键词： Bimetal/bimetallic Two-dimensional/2D Oxygen evolution Electrocatalytic MOF LDH

A hierarchically structured tin-cobalt composite with an enhanced electronic effect for high-performance CO_(2) electroreduction in a wide potential range

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Journal of Energy Chemistry 2023年第1期76卷 462-469,I0012页

作者： Xingxing Jiang Xuan Li Yan Kong Chen Deng Xiaojie Li Qi Hu hengpan Yang chuanxin he Institute of Microscale Optoelectronics College of Chemistry and Environmental EngineeringShenzhen UniversityShenzhen 518060GuangdongChina

Earth-abundant and nontoxic Sn-based materials have been regarded as promising catalysts for the electrochemical conversion of CO_(2)to C1 products,e.g.,CO and ***,it is still difficult for Snbased materials to obtain satisfactory performance at low-to-moderate ***,a simple and facile electrospinning technique is utilized to prepare a composite of a bimetallic Sn-Co oxide/carbon matrix with a hollow nanotube structure(Sn Co-HNT).Sn Co-HNT can maintain>90%faradaic efficiencies for C1 products within a wide potential range from-0.6 VRhe to-1.2 VRhe,and a highest 94.1%selectivity towards CO in an H-type ***,a 91.2%faradaic efficiency with a 241.3 m A cm^(-2)partial current density for C1 products could be achieved using a flow *** to theoretical calculations,the fusing of Sn/Co oxides on the carbon matrix accelerates electron transfer at the atomic level,causing electron deficiency of Sn centers and reversible variation between Co^(2+)and Co^(3+)*** synergistic effect of the Sn/Co composition improves the electron affinity of the catalyst surface,which is conducive to the adsorption and stabilization of key intermediates and eventually increases the catalytic activity in CO_(2)*** study could provide a new strategy for the construction of oxide-derived catalysts for CO_(2)electroreduction.

关键词： Hierarchic structure Tin-cobalt bimetallic oxide Electronic effect CO_(2)electroreduction Wide potential range

Janus heterostructure of cobalt and iron oxide as dual-functional electrocatalysts for overall water splitting

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Nano Research 2023年第2期16卷 2245-2251页

作者： Xiaojie Li Huike Zhang Xuan Li Qi Hu Chen Deng Xingxing Jiang hengpan Yang chuanxin he College of Chemistry and Environmental Engineering Shenzhen UniversityShenzhen 518060China Institute of Microscale Optoelectronics Shenzhen UniversityShenzhen 518060China

In electrocatalytic water splitting,low-cost dual-functional catalysts can not only reduce costs but also avoid cross-contamination of cathode and ***,the orderly aggregation of active sites for hydrogen evolution reaction(heR)and oxygen evolution reaction(OER)into a specific catalyst is very *** this study,a Co/Fe_(3)O_(4)Janus heterojunction supported on carbon fiber paper(J-CoFe-CFP)is designed and successfully ***,Co-Fe oxides have preferable OER activity but weak heR ***,in J-CoFe-CFP,due to the intense and special electronic interaction of different substances(Co and Fe3O4)in the Janus heterogeneous interface,a huge number of tidy high-quality heR and OER active sites are uniformly distributed on the interface simultaneously,which endows the catalyst with both excellent heR and OER *** heR,the overpotential@10 mA·cm^(−2)(ηheR)is only 53.9 mV,and the Tafel slope is 43.7 mV·dec^(−1).In OER,theηis 272 mV,and the Tafel slope is 50.2 mV·dec^(−1),much lower than those of RuO_(2)/*** the J-CoFe-CFP||J-CoFe-CFP two-electrode system,the required voltage is only 1.26 V at the beginning and 1.56 V@10 mA·cm^(−2),much lower than those of RuO_(2)/CFP||20%Pt/C/*** work provides a Janus heterojunction pathway for bifunctional water electrolysis catalysts.

关键词： Janus bifunctional electrocatalytic water splitting CoFe

Construction of cobalt-copper bimetallic oxide heterogeneous nanotubes for high-efficient and low-overpotential electrochemical CO_(2) reduction

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Journal of Energy Chemistry 2021年第3期30卷 1-6页

作者： Zhong Cheng Xiaodeng Wang hengpan Yang Xinyao Yu Qing Lin Qi Hu chuanxin he College of Chemistry and Environmental Engineering Shenzhen UniversityShenzhen 518060GuangdongChina

Currently,global warming and energy problems become more and more serious with the development of economy and the continuous consumption of fossil fuel,which are due to the release of greenhouse gas in the process of ... 详细信息

关键词： CO_(2)reduction reaction Electrocatalysts Bimetal Nanotube Selectivity