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Surface engineering of 1D nanocatalysts for value-added selective electrooxidation of organic chemicals

Nano Research 2024年第3期17卷 1327-1336页

作者： Yongping Yang Chuhao Liu Tinglu Song Mufan Li 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 TechnologyBeijing 100081China beijing National laboratory for Molecular Sciences College of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China

Electrolytic water splitting by renewable energy is a technology with great potential for producing hydrogen(H_(2))without carbon emission,but this technical route is hindered by its huge energy(electricity)cost,which is mainly wasted by the anode oxygen evolution reaction(OER)while the value of the anode product(oxygen)is very limited.Replacing the high-energy-cost OER with a selective organic compound electrooxidation carried out at a relatively lower potential can reduce the electricity cost while producing value-added chemicals.Currently,H_(2) generation coupled with synthesis of value-added organic compounds faces the challenge of low selectivity and slow generation rate of the anodic products.One-dimensional(1D)nanocatalysts with a unique morphology,well-defined active sites,and good electron conductivity have shown excellent performance in many electrocatalytic reactions.The rational design and regulation of 1D nanocatalysts through surface engineering can optimize the adsorption energy of intermediate molecules and improve the selectivity of organic electrooxidation reactions.Herein,we summarized the recent research progress of 1D nanocatalysts applied in different organic electrooxidation reactions and introduced several different fabrication strategies for surface engineering of 1D nanocatalysts.Then,we focused on the relationship between surface engineering and the selectivity of organic electrooxidation reaction products.Finally,future challenges and development prospects of 1D nanocatalysts in the coupled system consisting of organic electrooxidation and hydrogen evolution reactions are briefly outlined.

关键词： hydrogen generation organic compound electrooxidation one-dimensional(1D)nanocatalysts surface engineering selectivity

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Silicon dioxide-protection boosting the peroxidase-like activity of Fe single-atom catalyst for combining chemo-photothermal therapy

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Nano Research 2024年第6期17卷 4924-4933页

作者： Yu Fan Yu Yi Hongpan Rong Jiatao Zhang beijing key laboratory of construction-tailorable advanced functional materials and green applications School of Materials Science&EngineeringBeijing Institute of TechnologyBeijing 100081China CAS Center for Excellence in Nanoscience CAS KeyLaboratory for Biomedical Effects of Nanomaterials and NanosafetyNational Center for Nanoscience and Technology(NCNST)Beijing 100190China key laboratory of Medical Molecule Science and Pharmaceutics Engineering Ministry of Industry and Information TechnologySchool of Chemistry&Chemical EngineeringBeijing Key Laboratory of Construction-Tailorable Advanced Functional Materials and Green ApplicationsSchool of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081China

Carbon-based single-atom catalysts(SACs)have been widely studied in the field of biomedicine due to their excellent catalytic performance.However,carbon-based SACs usually aggregate during pyrolysis,which leads to the reduction of catalytic activity.Here,we describe a method to improve the monodispersion of SACs using silicon dioxide as a protective layer.The decoration of silicon dioxide serves as a buffer layer for individual nanoparticles,which is not destroyed during the pyrolysis process,ensuring the single-particle dispersion of the nanoparticles after etching.This approach increased the hydroxyl groups on the surface of Fe-SAC(Fe-SAC-SE)and improved its water solubility,resulting in a four times enhancement of the peroxidase(POD)-like activity of Fe-SAC-SE(58.4 U/mg)than that of non-protected SACs(13.9 U/mg).The SiO_(2)-protection approach could also improve the catalytic activities of SACs with other metals such as Mn,Co,Ni,and Cu,indicating its generality for SACs preparation.Taking advantage of the high POD-like activity,photothermal properties,and large specific surface area of Fe-SAC-SE,we constructed a synergistic therapeutic system(Fe-SAC-SE@DOX@PEG)for combining the photothermal therapy,catalytic therapy,and chemotherapy.It was verified that the photothermal properties of Fe-SAC-SE@DOX@PEG could effectively improve its POD-like activity,exhibiting excellent tumor-killing performance at the cellular level.This work may provide a general approach to improve the performances of SACs for disease therapy and diagnosis.

关键词： single-atom catalysts peroxidase-like activity SiO2-protection photothermal therapy catalytic therapy chemotherapy

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Constructing inter-diffusive PtCuNi/WO_(3)interface to enhance the catalytic activity and stability in oxygen reduction

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Tungsten 2024年第2期6卷 293-303页

作者： Hao-Zhe Xu Dong Li Ying Chen Pin Fang Xiao-Xing Ke Olga Demidenko Yu-Jing Li beijing key laboratory of construction tailorable advanced functional materials and green applications Experimental Center of Advanced MaterialsSchool of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081China Faculty of materials and Manufacturing Beijing University of TechnologyBeijing 100124China Scientifi c-Practical materials Research Centre National Academy of Sciences of Belarus220072 MinskBelarus

Platinum-group-metal-based alloy nanocrystals have been considered as the most effi cient catalysts for oxygen reduction reaction(ORR).However,the poor stability issues limit their further deployment in industrialization.Tungsten oxide(WO_(3))has received attention due to its intrinsic electrochemical stability and proton absorption/desorption capability.In this work,we prepared PtCuNi/WO_(3)/C hybrid catalyst with inter-diff usive alloy/WO_(3)interface on carbon.The catalyst exhibits enhanced activity and stability associated with the WO_(3)content.The characterization results suggest that the increased activity originates from the complementary proton supply of non-stoichiometric H_(x)WO_(3).Moreover,WO_(3)prevents the particle from dissolution and detachment under vigorous electrochemical polarizations.The enhanced stability originates from the electronic interaction established between Pt and W.This work provides new strategies to design high-performance ORR catalysts by taking the merits of WO_(3)。

关键词： Tungsten oxide PtCuNi Interface Electronic interaction

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Stability of dimensionally stable anode for chlorine evolution reaction

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Nano Research 2024年第3期17卷 949-959页

作者： Ziliang Deng Shuying Xu Chuhao Liu Xueqiang Zhang Mufan Li 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 TechnologyBeijing 100081China beijing National laboratory for Molecular Sciences College of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China Laser Micro/Nano-Fabrication laboratory School of Mechanical EngineeringBeijing Institute of TechnologyBeijing 10081China

Chlorine(Cl2)is one of the most important chemicals produced by the electrolysis of brine solutions and is a key raw material for many areas of industrial chemistry.For nearly half a century,dimensionally stable anode(DSA)made from a mixture of RuO_(2) and TiO_(2) solid oxides coated on Ti substrate has been the most widely used electrode for chlorine evolution reaction(CER).In harsh operating environments,the stability of DSAs remains a major challenge greatly affecting their lifetime.The deactivation of DSAs significantly increases the cost of the chlor-alkali industry due to the corrosion of Ru and the formation of the passivation layer TiO_(2).Therefore,it is urgent to develop catalysts with higher activity and stability,which requires a thorough understanding of the deactivation mechanism of DSA catalysts.This paper reviews existing references on the deactivation mechanisms of DSA catalysts,including both experimental and theoretical studies.Studies on how CER selectivity affects electrode stability are also discussed.Furthermore,studies on the effects of the preparation process,elemental composition,and surface/interface structures on the DSA stability and corresponding improvement strategies are summarized.The development of other non-DSA-type catalysts with comparable stability is also reviewed,and future opportunities in this exciting field are also outlined.

关键词： chlorine evolution reaction(CER) dimensionally stable anode(DSA) RuO_(2)-TiO_(2) metal oxide anode stability

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Phase-engineering modulation of Mn-based oxide cathode for constructing super-stable sodium storage

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Journal of Energy Chemistry 2024年第1期88卷 421-427,I0010页

作者： Quanqing Zhao Ruru Wang Ming Gao Bolin Liu Jianfeng Jia Haishun Wu Youqi Zhu Chuanbao Cao key laboratory of Magnetic Molecules and Magnetic Information materials of Ministry of Education School of Chemistry and Materials ScienceShanxi Normal UniversityTaiyuan 030032ShanxiChina Metals and Chemistry Research Institute China Academy of Railway Sciences Corporation LimitedBeijing 100081China Research Center of materials Science Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green ApplicationsBeijing Institute of TechnologyBeijing 100081China

The Mn-based oxide cathode with enriched crystal phase structure and component diversity can provide the excellent chemistry structure for Na-ion batteries.Nevertheless,the broad application prospect is obstructed by the sluggish Na^(+)kinetics and the phase transitions upon cycling.Herein,we establish the thermodynamically stable phase diagram of various Mn-based oxide composites precisely controlled by sodium content tailoring strategy coupling with co-doping and solid-state reaction.The chemical environment of the P2/P'3 and P2/P3 biphasic composites indicate that the charge compensation mechanism stems from the cooperative contribution of anions and cations.Benefiting from the no phase transition to scavenge the structure strain,P2/P'3 electrode can deliver long cycling stability(capacity retention of 73.8%after 1000 cycles at 10 C)and outstanding rate properties(the discharge capacity of 84.08 mA h g^(-1)at 20 C)than P2/P3 electrode.Furthermore,the DFT calculation demonstrates that the introducing novel P'3 phase can significantly regulate the Na^(+)reaction dynamics and modify the local electron configuration of Mn.The effective phase engineering can provide a reference for designing other high-performance electrode materials for Na-ion batteries.

关键词： Sodium ion battery Oxide cathode Phase engineering Phase diagram Na~+kinetic

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Interfacial engineering of the layered oxide cathode materials for sodium-ion battery

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Nano Research 2024年第3期17卷 1441-1464页

作者： Quanqing Zhao Ruru Wang Ming Gao Faheem KButt Jianfeng Jia Haishun Wu Youqi Zhu key laboratory of Magnetic Molecules and Magnetic Information materials of Ministry of Education School of Chemistry and Materials ScienceShanxi Normal UniversityTaiyuan 030032China Metals and Chemistry Research Institute China Academy of Railway Sciences Corporation LimitedBeijing 100081China Department of Physics Division of Science and TechnologyUniversity of EducationLahore 54770Pakistan Research Center of materials Science Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green ApplicationsBeijing Institute of TechnologyBeijing 100081China

The layered metal oxides are reviewed as the hopeful cathode materials for high-performance sodium-ion batteries(SIBs)due to their large theoretical capacity,favorable two-dimensional(2D)ion diffusion channel,and simple manipuility.However,their cycling stability,rate capability,and thermal stability are still significantly concerned and highlighted before further practical application.The chemical,mechanical and electrochemical stability of the cathode–electrolyte interfaces upon cycling is of great significance.Herein,the unique structural and electrochemical properties of the layered oxide cathode materials for SIB are reviewed.The mechanism of bulk/surface degradation induced by oxygen evolution,phase transition,microcrack,and electrolyte decomposition is thoroughly understood.Furthermore,the interfacial engineering to construct stable interface through various effective methods is fully discussed.The future outlook and challenges for interfacial engineering in this filed are also summarized.This review should shed light on the rational design and construct of robust interface for applications of superior layered oxide cathodes in SIB and may suggest future research directions.

关键词： interfacial engineering sodium-ion battery layered oxide electrolyte interface

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空间选择性缺陷管理制备高性能碳基CsPbI_(3)钙钛矿太阳能电池

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Science Bulletin 2024年第8期69卷 1050-1060页

作者：王海亮张啟先林则东刘慧丛魏晓震宋永发律春宇李卫平朱立群王科翔崔振华王兰林常青殷鹏刚宋廷鲁白阳陈棋杨世和陈海宁 School of materials Science and Engineering Beihang UniversityBeijing 100191China Guangdong Provincial key Lab of Nano-Micro materials Research School of Advanced MaterialsShenzhen Graduate SchoolPeking UniversityShenzhen 518055China Institute of Biomedical Engineering Shenzhen Bay LaboratoryShenzhen 518107China School of Chemistry Beihang UniversityBeijing 100191China beijing key laboratory of construction tailorable advanced functional materials and green applications MIIT Key Laboratory for Low-Dimensional Quantum Structure and DevicesExperimental Center of Advanced MaterialsSchool of Materials Science&EngineeringBeijing Institute of TechnologyBeijing 100081China School of Internet of Things Engineering Jiangnan UniversityWuxi 214122China School of Physical Science and Technology Guangxi UniversityNanning 530004China Experimental Center of advanced materials School of Materials Science&EngineeringBeijing Institute of TechnologyBeijing 100081China

Defects formed at the surface,buried interface and grain boundaries(GB)of CsPbI_(3)perovskite films considerably limit photovoltaic performance.Such defects could be passivated effectively by the most prevalent post modification strategy without compromising the photoelectric properties of perovskite films,but it is still a great challenge to make this strategy comprehensive to different defects spatially distributed throughout the films.Herein,a spatially selective defect management(SSDM)strategy is developed to roundly passivate various defects at different locations within the perovskite film by a facile one-step treatment procedure using a piperazine-1,4-diium tetrafluoroborate(PZD(BF_(4))_(2))solution.The small-size PZD^(2+)cations could penetrate into the film interior and even make it all the way to the buried interface of CsPbI_(3)perovskite films,while the BF_(4)^(-)anions,with largely different properties from I^(-)anions,mainly anchor on the film surface.Consequently,virtually all the defects at the surface,buried interface and grain boundaries of CsPbI_(3)perovskite films are effectively healed,leading to significantly improved film quality,enhanced phase stability,optimized energy level alignment and promoted carrier transport.With these films,the fabricated CsPbI_(3)PSCs based on carbon electrode(C-PSCs)achieve an efficiency of18.27%,which is among the highest-reported values for inorganic C-PSCs,and stability of 500 h at 85℃with 65%efficiency maintenance.

关键词： CsPbI_(3) Defects Spatially selective defect management Carbon electrode

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Symmetry breaking of highly symmetrical nanoclusters for triggering highly optical activity

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Fundamental Research 2024年第1期4卷 63-68页

作者： Xiao Wei Hao Li Honglei Shen Chuanjun Zhou Shuxin Wang Xi Kang Manzhou Zhu Department of Chemistry and Centre for Atomic Engineering of advanced materials Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of EducationInstitutes of Physical Science and Information Technology and Anhui Province Key Laboratory of Chemistry for Inorganic/Organic Hybrid Functionalized Materials.Anhui UniversityHefei 230601China

Developing new approaches to fulfill the enantioseparation of nanocluster racemates and construct cluster-based nanomaterials with optical activity remains highly desired in cluster science,because it is an essential prerequisite for fundamental research and extensive applications of these nanomaterials.We herein propose a strategy termed“active-site exposing and partly re-protecting”to trigger the symmetry breaking of highly symmetrical nanoclusters and to render cluster crystals optically active.The vertex PPh_(3)of the symmetrical Ag_(29)(SSR)_(12)(PPh_(3))_(4)(SSR=1,3-benzenedithiol)nanocluster was firstly dissociated in the presence of counterions with large steric hindrance,and then the exposed Ag active sites of the obtained Ag_(29)(SSR)_(12)nanocluster were partly re-protected by Ag^(+),yielding an Ag_(29)(SSR)_(12)-Ag_(2)nanocluster with a symmetry-breaking construction.Ag_(29)(SSR)_(12)-Ag_(2)followed a chiral crystallization mode,and its crystal displayed strong optical activity,derived from CD and CPL characterizations.Overall,this work presents a new approach(i.e.,active-site exposing and partly re-protecting)for the symmetry breaking of highly symmetrical nanoclusters,the enantioseparation of nanocluster racemates,and the achievement of highly optical activity.

关键词： Atomically precise nanocluster Symmetry breaking Enantioseparation Circularly polarized luminescent Photoluminescence

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A post-modification strategy to precisely construct dual-atom sites for oxygen reduction electrocatalysis

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Journal of Energy Chemistry 2024年第3期90卷 511-517,I0012页

作者： Juan Wang Xinyan Liu Chang-Xin Zhao Yun-Wei Song Jia-Ning Liu Xi-Yao Li Chen-Xi Bi Xin Wan Jianglan Shui Hong-Jie Peng Bo-Quan Li Jia-Qi Huang School of materials Science and Engineering Beijing Institute of TechnologyBeijing 100081China advanced Research Institute of Multidisciplinary Science Beijing Institute of TechnologyBeijing 100081China beijing key laboratory of green Chemical Reaction Engineering and Technology Department of Chemical EngineeringTsinghua UniversityBeijing 100084China Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of ChinaChengdu 611731SichuanChina School of materials Science and Engineering Beihang UniversityBeijing 100191China

Dual-atom catalysts(DACs) afford promising potential for oxygen reduction electrocatalysis due to their high atomic efficiency and high intrinsic activity.However,precise construction of dual-atom sites remains a challenge.In this work,a post-modification strategy is proposed to precisely fabricate DACs for oxygen reduction electrocatalysis.Concretely,a secondary metal precursor is introduced to the primary single-atom sites to introduce direct metal-metal interaction,which ensures the formation of desired atom pair structure during the subsequent pyrolysis process and allows for successful construction of DACs.The as-prepared FeCo-NC DAC exhibits superior oxygen reduction electrocatalytic activity with a half-wave potential of 0,91 V vs.reversible hydrogen electrode.Zn-air batteries equipped with the FeCo-NC DAC demonstrate higher peak power density than those with the Pt/C benchmark.More importantly,this post-modification strategy is demonstrated universal to achieve a variety of dual-atom sites.This work presents an effective synthesis methodology for precise construction of catalytic materials and propels their applications in energy-related devices.

关键词： Dual-atom catalysts Electrocatalysis Oxygen reduction reaction Post-modification Zinc–air batteries

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High-throughput calculation-based rational design of Fe-doped MoS_(2) nanosheets for electrocatalytic p H-universal overall water splitting

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Journal of Energy Chemistry 2024年第4期91卷 194-202页

作者： Guangtong Hai Xiangdong Xue Zhenyu Wu Canyang Zhang Xin Liu Xiubing Huang Institute of Zhejiang University-Quzhou Zhejiang UniversityQuzhou 324000ZhejiangChina beijing key laboratory of Membrane materials and Engineering Department of Chemical EngineeringTsinghua UniversityBeijing 100084China beijing advanced Innovation Center for materials Genome Engineering Beijing Key Laboratory of Function Materials for Molecule&Structure ConstructionSchool of Materials Science and EngineeringUniversity of Science and TechnologyBeijing 100083China CentreÉnergie Matériaux et Télécommunications(EMT) Institut national de la recherche scientifique(INRS)Varennes J3X1P7QuébecCanada

Electrocatalytic water splitting is crucial for H2generation via hydrogen evolution reaction(HER)but subject to the sluggish dynamics of oxygen evolution reaction(OER).In this work,single Fe atomdoped MoS_(2)nanosheets(SFe-DMNs)were prepared based on the high-throughput density functional theory(DFT)calculation screening.Due to the synergistic effect between Fe atom and MoS_(2)and optimized intermediate binding energy,the SFe-DMNs could deliver outstanding activity for both HER and OER.When assembled into a two-electrode electrolytic cell,the SFe-DMNs could achieve the current density of 50 mA cm^(-2)at a low cell voltage of 1.55 V under neutral condition.These results not only confirmed the effectiveness of high-throughput screening,but also revealed the excellent activity and thus the potential applications in fuel cells of SFe-DMNs.

关键词： High-throughput calculation Overall water splitting Single atom doped catalyst Molybdenum disulfide nanosheet

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