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Strain‑Induced Surface Interface Dual Polarization Constructs PML‑Cu/Bi_(12)O_(17)Br_(2) High‑Density active sites for CO_(2) Photoreduction

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Nano-Micro Letters 2024年第5期16卷 169-183页

作者： Yi Zhang Fangyu Guo Jun Di Keke Wang Molly Meng‑Jung Li Jiayu Dai Yuanbin She Jiexiang Xia Huaming Li School of Chemistry and Chemical Engineering Institute for Energy ResearchSchool of the Environment and Safety EngineeringJiangsu UniversityZhenjiang 212013People’s Republic of China State Key Laboratory Breeding Base of Green Chemistry‑Synthesis Technology College of Chemical EngineeringZhejiang University of TechnologyHangzhou 310014People’s Republic of China College of Science and Hunan Key Laboratory of Extreme Matter and ApplicationsNational University of Defense TechnologyChangsha 410073People’s Republic of China Department of Applied Physics The Hong Kong Polytechnic UniversityHung HomHong KongPeople’s Republic of China School of Chemistry and Chemical Engineering National Special Superfine Powder Engineering Research CenterNanjing University of Science and TechnologyNanjing 210094People’s Republic of China Key Laboratory of the Ministry of Education for Advanced Catalysis Materials Zhejiang Normal UniversityJinhua 321004People’s Republic of China

The insufficient active sites and slow interfacial charge trans-fer of photocatalysts restrict the efficiency of CO_(2) photoreduction.The synchronized modulation of the above key issues is demanding and chal-lenging.Herein,strain-induced strategy is developed to construct the Bi–O-bonded interface in Cu porphyrin-based monoatomic layer(PML-Cu)and Bi_(12)O_(17)Br_(2)(BOB),which triggers the surface interface dual polarization of PML-Cu/BOB(PBOB).In this multi-step polarization,the built-in electric field formed between the interfaces induces the electron transfer from con-duction band(CB)of BOB to CB of PML-Cu and suppresses its reverse migration.Moreover,the surface polarization of PML-Cu further promotes the electron converge in Cu atoms.The introduction of PML-Cu endows a high density of dispersed Cu active sites on the surface of PBOB,significantly promoting the adsorption and activation of CO_(2) and CO desorption.The conversion rate of CO_(2) photoreduction to CO for PBOB can reach 584.3μmol g-1,which is 7.83 times higher than BOB and 20.01 times than PML-Cu.This work offers valuable insights into multi-step polarization regulation and active site design for catalysts.

关键词： Bi_(12)O_(17)Br_(2) Porphyrin CO_(2)photoreduction Polarization active sites

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Construction of electron rich Fe active sites by FeCu alloy anchoring on carbon nitride for photocatalytic nitrogen reduction

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Rare Metals 2024年第4期43卷 1570-1579页

作者： Gang Dong Cong Huang Fei-Yang Chen Xue-Qin Liu Zhen Li Xiao-Li Su Tao Zeng Yun-Xia Chen Yi-Huang Chen Yang Wang School of Materials Science and Engineering Jingdezhen Ceramic University Faculty of Materials Science and Chemistry China University of Geosciences College of Chemistry and Materials Engineering Wenzhou University

Given the clean and inexhaustible solar energy from solar light,photocatalytic ammonia synthesis is extremely appealing.However,high electron-hole recombination rates and insufficient active sites severely limited N2 photoreaction reduction.Herein,we designed and fabricated FeCu alloy nanoparticles anchored on carbon nitride nanosheets with excellent photocatalyt ic ammonia synthesis performance.As a coupler between Fe and carbon nitride,Cu promotes the separation of photogenerated charge carriers in carbon nitride under solar light irradiation,and renters the semiconductor a forceful electron donor for the Fe active sites.The accumulated electrons at Fe sites furtherly facilitated the adsorption and activation of the molecular nitrogen.Besides,the uniform dispersed FeCu alloy nanoparticles were on carbon nitride nanosheets enhanced the stability of photocataly tic nitrogen reduction reaction,making the artificial photocataly tic ammonia synthesis more sustainable for application.This work highlights that a direct electron transfer channel can be used to regulate the photochemical nitrogen fixation network.

关键词： Photocatalytic N 2 fixation Carbon nitride FeCu alloy active sites Hydrogenation pathway

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A Review of In‑Situ Techniques for Probing active sites and Mechanisms of Electrocatalytic Oxygen Reduction Reactions

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Nano-Micro Letters 2023年第2期15卷 61-113页

作者： Jinyu Zhao Jie Lian Zhenxin Zhao Xiaomin Wang Jiujun Zhang College of Materials Science and Engineering Taiyuan University of TechnologyTaiyuan 030024People’s Republic of China Institute for Sustainable Energy/College of Sciences Shanghai UniversityShanghai 200444People’s Republic of China

Electrocatalytic oxygen reduction reaction(ORR)is one of the most important reactions in electrochemical energy technologies such as fuel cells and metal–O2/air batteries,etc.However,the essential catalysts to overcome its slow reaction kinetic always undergo a complex dynamic evolution in the actual catalytic process,and the concomitant intermediates and catalytic products also occur continuous conversion and reconstruction.This makes them difficult to be accurately captured,making the identification of ORR active sites and the elucidation of ORR mechanisms difficult.Thus,it is necessary to use extensive in-situ characterization techniques to proceed the real-time monitoring of the catalyst structure and the evolution state of intermediates and products during ORR.This work reviews the major advances in the use of various in-situ techniques to characterize the catalytic processes of various catalysts.Specifically,the catalyst structure evolutions revealed directly by in-situ techniques are systematically summarized,such as phase,valence,electronic transfer,coordination,and spin states varies.In-situ revelation of intermediate adsorption/desorption behavior,and the real-time monitoring of the product nucleation,growth,and reconstruction evolution are equally emphasized in the discussion.Other interference factors,as well as in-situ signal assignment with the aid of theoretical calculations,are also covered.Finally,some major challenges and prospects of in-situ techniques for future catalysts research in the ORR process are proposed.

关键词： Oxygen reduction reaction Catalysts In-situ techniques active sites Mechanisms

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Hollow catalysts through different etching treatments to improve active sites and oxygen vacancies for high-performance Li-O_(2)battery

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Nano Research 2023年第5期16卷 6798-6804页

作者： Jiachen Qiu Yuran Lin Shuting Zhang Jie Ma Yu Zhang Mengwei Yuan Genban Sun Caiyun Nan Beijing Key Laboratory of Energy Conversion and Storage Materials College of ChemistryBeijing Normal UniversityBeijing 100875China Center for Advanced Materials Research Beijing Normal UniversityZhuhai 519087China Department of Chemistry Tsinghua UniversityBeijing 100084China

Li-O_(2)batteries are regarded as one of the most promising next-generation battery systems due to their high theoretical energy density,finding effective cathode catalysts with fine-tuned structure is a key way to improve the performance.Herein,based on the structure of cubic zeolitic imidazolate framework-67(ZIF-67),a series of hollow catalysts were synthesized by different chemical etching treatments.Firstly,from the perspective of metal,nickel nitrate is used for etching,hollow Ni ZIF is obtained through Kirkendall effect.Secondly,hollow TA-ZIF is obtained by adding tannic acid to replace the methylimidazole ligand.Hollow structures have larger surface areas,materials can expose more active sites,which can lead to better performance of Li-O_(2)batteries.On this basis,having more oxygen vacancies can also improve the battery performance.At the same time,further loading noble metal ruthenium on the synthesized cobalt-based catalyst can effectively reduce the overpotential of Li-O_(2)battery and improve the battery performance.For TA-ZIF with more stable hollow structure and more oxygen vacancies,the cycle performance reaches 330 cycles after loading Ru.Compared with the 64 cycles of solid Co_(3)O_(4),it has a great improvement.

关键词： hollow structure active sites oxygen vacancies noble metal cathode catalyst Li-O_(2)battery

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Trimetallic oxyhydroxides as active sites for large-current-density alkaline oxygen evolution and overall water splitting

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Journal of Materials Science & Technology 2022年第15期110卷 128-135页

作者： Lei Chen Yunpeng Wang Xin Zhao Yuchao Wang Qian Li Qichen Wang Yougen Tang Yongpeng Lei State Key Laboratory of Powder Metallurgy Hunan Key Laboratory of Two-Dimensional MaterialsCentral South UniversityChangsha 410083China Hunan Provincial Key Laboratory of Chemical Power Sources College of Chemistry and Chemical EngineeringCentral South UniversityChangsha 410083China School of Physics and Electronics Hunan Key Laboratory for Super-micro structure and Ultrafast ProcessCentral South UniversityChangsha 410083China

Earth-abundant electrocatalysts for large-current-density water splitting under alkaline condition are desirable.Oxygen evolution reaction,which is a bottleneck of the overall water splitting,faces the problems of complicated reconstruction and deficiency in rational design of active sites.Herein,we report a series of transition metal chalcogenides for alkaline OER.Among them,FeCoNi(S)displayed a low overpotential of 293 m V to deliver a current density of 500 m A cm^(-2),which is in the top level of non-precious metal based OER electrocatalysts.A combination of(ex)in situ characterizations and DFT calculation shows that Ni(Fe,Co)trimetallic oxyhydroxides were the active sites for highly-efficient OER.Furthermore,for FeCoNi(S),when used as a bifunctional catalyst for water splitting,it only required a cell voltage of 1.84 V to deliver~500 m A cm^(-2) with extraordinary long-term stability over 2000 h.This work provides the comprehension of high-efficiency,robust catalysts for OER and overall water splitting at large current densities in alkaline media.

关键词： Oxygen evolution active sites Surface reconstruction Large current density Overall water splitting

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Exploring the catalytic function and active sites of a novel C-glycosyltransferase from Anemarrhena asphodeloides

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Synthetic and Systems Biotechnology 2022年第1期7卷 621-630页

作者： Jia Huang Yaru She Jingyang Yue Yidu Chen Yu Li Jing Li Yonger Hu Deying Yang Jiabo Chen Lu Yang Zhongqiu Liu Ruibo Wu Pengfei Jin Lixin Duan Joint Laboratory for Translational Cancer Research of Chinese Medicine of the Ministry of Education of the People’s Republic of China International Institute for Translational Chinese MedicineGuangzhou University of Chinese MedicineGuangzhou510006PR China Guangdong Provincial Key Laboratory of New Drug Design and Evaluation School of Pharmaceutical SciencesSun Yat-sen UniversityGuangzhou510006PR China Department of Pharmacy Beijing HospitalNational Center of GerontologyInstitute of Geriatric MedicineChinese Academy of Medical SciencesBeijing Key Laboratory of Assessment of Clinical Drugs Risk and Individual Application(Beijing Hospital)Beijing100730PR China

Anemarrhena asphodeloides is an immensely popular medicinal herb in China,which contains an abundant of mangiferin.As an important bioactive xanthone C-glycoside,mangiferin possesses a variety of pharmacological activities and is derived from the cyclization reaction of a benzophenone C-glycoside(maclurin).Biosyntheti-cally,C-glycosyltransferases are critical for the formation of benzophenone C-glycosides.However,the benzo-phenone C-glycosyltransferases from Anemarrhena asphodeloides have not been discovered.Herein,a promiscuous C-glycosyltransferase(AaCGT)was identified from Anemarrhena asphodeloides.It was able to catalyze efficiently mono-C-glycosylation of benzophenone,together with di-C-glycosylation of dihydrochalcone.It also exhibited the weak O-glycosylation or potent S-glycosylation capacities toward 12 other types of flavonoid scaffolds and a simple aromatic compound with–SH group.Homology modeling and mutagenesis experiments revealed that the glycosylation reaction of AaCGT was initiated by the conserved residue H23 as the catalytic base.Three critical residues H356,W359 and D380 were involved in the recognition of sugar donor through hydrogen-bonding interactions.In particular,the double mutant of F94W/L378M led to an unexpected enzy-matic conversion of mono-C-to di-C-glycosylation.This study highlights the important value of AaCGT as a potential biocatalyst for efficiently synthesizing high-value C-glycosides.

关键词： C-glycosides Anemarrhena asphodeloides C-glycosyltransferases Benzophenone active sites

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In situ identification of active sites during electrocatalytic hydrogen evolution

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Nano Research 2023年第12期16卷 12910-12918页

作者： Dongge Wang Juanxia Wu Liying Jiao Liming Xie CAS Key Laboratory of Standardization and Measurement for Nanotechnology National Center for Nanoscience and TechnologyBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China Key Laboratory of Organic Optoelectronics and Molecular Engineering of the Ministry of Education Department of ChemistryTsinghua UniversityBeijing 100084China

The rational design of efficient,low cost,and durable catalysts is critical for the industrial applications of electrocatalytic hydrogen production.A key step towards the structure design of high-performance catalysts for hydrogen evolution reaction(HER)relies on the in situ identification of the catalytic active sites in the process of HER,which is of great challenge.In this review,we summarize the recent advances on the in situ investigation of the active sites on low dimensional catalysts for HER.We highlight the characterization techniques used for this purpose,including scanning electrochemical microscopy(SECM),scanning electrochemical cell microscopy(SECCM),electrochemical scanning tunneling microscopy(EC-STM),in situ liquid phase transmission electron microscopy(LP-TEM),and in situ spectroscopic tools.We conclude with an overview of the main technical limitations for the current approaches and give an outlook to future opportunities in this emerging field.

关键词： in situ hydrogen evolution reaction active sites electrocatalyst

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Morphology effects in MnCeO_(x)solid solution-catalyzed NO reduction with CO:active sites,water tolerance,reaction pathway

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Nano Research 2023年第5期16卷 6951-6959页

作者： Quanquan Shi Yifei Zhang Zhiwen Li Zhongkang Han Liangliang Xu Alfons Baiker Gao Li College of Science&College of Material Science and Art Design Inner Mongolia Agricultural UniversityHohhot 010018China College of Chemistry and Chemical Engineering Shenyang Normal UniversityShenyang 110034China State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China School of Materials Science and Engineering Zhejiang UniversityHangzhou 310027China Department of Chemical and Biomolecular Engineering Korea Advanced Institute of Science and TechnologyDaejeon 34141Republic of Korea Department of Chemistry and Applied Biosciences Institute for Chemical and BioengineeringETH ZurichHönggerbergHClCH-8093 ZurichSwitzerland

Morphological effects of nanoparticles are crucial in many solid-catalyzed chemical transformations.We herein prepared two manganese-ceria solid solutions,well-defined MnCeO_(x)nanorods and MnCeO_(x)-nanocubes,exposing preferentially(111)and(100)facets of ceria,respectively.The incorporation of Mn dopant into ceria lattice strongly enhanced the catalytic performance in the NO reduction with CO.MnCeO_(x)(111)catalyst outperformed MnCeO_(x)(100)counterpart due to its higher population density of oxygen vacancy defects.In-situ infrared spectroscopy investigations indicated that the reaction pathway over MnCeO_(x)and pristine CeO_(2)is similar and that besides the direct pathway,an indirect pathway via adsorbed hyponitrite as an intermediate cannot be ruled out.X-ray photoelectron and Raman spectroscopies as well as first-principles density functional theory(DFT)calculations indicate that the enhanced catalytic performance of MnCeO_(x)can be traced back to its“Mn–OL(VÖ)–Mn–OL(VÖ)–Ce”connectivities.The Mn dopant strongly facilitates the formation of surface oxygen vacancies(VÖ)by liberating surface lattice oxygen(OL)via CO*+OL→CO_(2)*+VÖand promotes the reduction of NO,according to NO*+VÖ→N*+OL and 2N*→N_(2).The Mn dopant impact on both the adsorption of CO and activation of OL reveals that a balance between these two effects is critical for facilitating all reaction steps.

关键词： NO reduction with CO manganese-ceria solid solution morphology effects reaction mechanism active sites

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The active sites and Corresponding Stability Challenges of the M-N-C Catalysts for Proton Exchange Membrane Fuel Cell

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Chinese Journal of Chemistry 2023年第6期41卷 710-724页

作者： Ruolin Peng Zhongkun Zhao Hongmin Sun Yongping Yang Tinglu Song Yao Yang Jiankun Shao Haibo Jin Hongtao Sun Zipeng Zhao Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Applications Experimental Center of Advanced MaterialsSchool of Materials Science and EngineeringBeijing Institute of TechnologyBeijing100081China The Harold and Inge Marcus Department of Industrial and Manufacturing Engineering The Pennsylvania State UniversityUniversity ParkPA16802-4400USA School of Engineering Westlake UniversityHangzhouZhejiang 310030China State Key Laboratory of Explosion Science and Technology Bejing Institute of TechnologyBeijing 100081China The Materials Research institute The Pennsylvania State UniversityUniversityParkPA16802-4400UA

Proton exchange membrane fuel cells(PEMFCs)as promising alternatives to traditional internal combustion engines have attracted massive concerns to promote their wide application in society.However,the biggest challenge to the commercialization of PEMFCs remains the high cost due to the adoption of the platinum group metal(PGM)catalysts in the cathode.

关键词： Proton exchange membrane fuel cell Electrocatalysis Oxygen reduction reaction M-N-C catalysts active sites Stability Degradation mechanisms

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Superior Iodine Uptake Capacity Enabled by an Open Metal-Sulfide Framework Composed of Three Types of active sites

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CCS Chemistry 2023年第7期5卷 1540-1548页

作者： Yugang Zhang Linwei He Tingting Pan Jian Xie Fuqi Wu Xinglong Dong Xia Wang Lixi Chen Shicheng Gong Wei Liu Litao Kang Junchang Chen Lanhua Chen Long Chen Yu Han Shuao Wang State Key Laboratory of Radiation Medicine and Protection School for Radiological and Interdisciplinary Sciences(RAD-X)Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education InstitutionsSoochow UniversitySuzhou 215123 Advanced Membranes and Porous Materials(AMPM)Center Physical Sciences and Engineering DivisionKing Abdullah University of Science and Technology(KAUST)Thuwal 23955-6900 School of Life Sciences School of Civil EngineeringShaoxing UniversityShaoxing 312000 School of Environmental and Materials Engineering Yantai UniversityYantai 264005

Efficient adsorption of gaseous radioiodine is pivotal for the sustainable development of nuclear energy and the long-termradiation safety of the ecological system.However,state-of-the-art adsorbents(e.***.metal-organic frameworks and covalent-organic frameworks)currently under exploration suffer severely from limited adsorption capacity,especially under a real-world scenariowith extremely lowradioiodine concentration and elevated temperature.This mostly originates from the relatively weak sorption driving forces mainly determinedby the iodine-adsorbent interaction consistingof noncovalent interactionswith a small fraction of strong chemical bonding.Here,we document the discovery of an open metal-sulfide framework((NH_(4))_(2)(Sn_(3)S_(7)),donated as SCU-SnS)constructed by three different types of active sites as a superior iodine adsorbent.Benefiting from the ability of iodine for pre-enrichment into the framework by charge-balancing NH_(4)^(+)through N-H···I interaction,the efficient reduction of I^(2)affording I^(-)by S^(2-),and extremely high binding affinity between Sn_(4)^(+)and I^(-),SCU-SnS exhibit a record-breaking iodine adsorption capacity(2.12 g/g)under dynamic breakthrough conditions and the highest static capacity(6.12 g/g)among all reported inorganic adsorbents,both at 348 K.Its facile synthesis and low cost endow SCU-SnS with powerful application potential for the nuclear industry.

关键词： iodine metal-sulfide framework removal active sites dynamic adsorptio

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