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A cascade of in situ conversion of bicarbonate to CO_(2) and CO_(2) electroreduction in a flow cell with a Ni-N-S catalyst

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Journal of Energy Chemistry 2024年第1期88卷 183-193,I0005页

作者： Linghui Kong Min Wang Yongxiao Tuo Shanshan Zhou Jinxiu Wang Guangbo Liu Xuejing Cui Jiali Wang Luhua Jiang nanomaterials and electrocatalysis laboratory College of Materials Science and EngineeringQingdao University of Science and TechnologyQingdao 266042ShandongChina State Key laboratory of Heavy Oil Processing College of New EnergyChina University of Petroleum(East China)Qingdao 266580ShandongChina

Combination of CO_(2) capture using inorganic alkali with subsequently electrochemical conversion of the resultant HCO_(3)^(-)to high-value chemicals is a promising route of low cost and high *** electrochemical reduction of HCO_(3)^(-)is challenging due to the inaccessible of negatively charged molecular groups to the electrode ***,we adopt a comprehensive strategy to tackle this challenge,i.e.,cascade of in situ chemical conversion of HCO_(3)^(-)to CO_(2) and CO_(2) electrochemical reduction in a flow *** a tailored Ni-N-S single atom catalyst(SACs),where sulfur(S)atoms located in the second shell of Ni center,the CO_(2)electroreduction(CO_(2)ER)to CO is *** experimental results and density functional theory(DFT)calculations reveal that the introduction of S increases the p electron density of N atoms near Ni atom,thereby stabilizing^(*)H over N and boosting the first proton coupled electron transfer process of CO_(2)ER,i.e.,^(*)+e^(-)+^(*)H+^(*)CO_(2)→^(*)*** a result,the obtained catalyst exhibits a high faradaic efficiency(FE_(CO)~98%)and a low overpotential of 425 mV for CO production as well as a superior turnover frequency(TOF)of 47397 h^(-1),outcompeting most of the reported Ni *** importantly,an extremely high FECOof 90%is achieved at 50 mA cm^(-2)in the designed membrane electrode assembly(MEA)cascade electrolyzer fed with liquid *** work not only highlights the significant role of the second coordination on the first coordination shell of the central metal for CO_(2)ER,but also provides an alternative and feasible strategy to realize the electrochemical conversion of HCO_(3)^(-)to high-value chemicals.

关键词： S doped Ni-N-C single atom catalysts CO_(2)electrochemical reduction DFT calculations Membrane electrode assembly Reduction of bicarbonate

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Recent advances in electrocatalysts for seawater splitting

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Nano Materials Science 2023年第1期5卷 101-116页

作者： Guangbo Liu Yingshuang Xu Teng Yang Luhua Jiang nanomaterial&electrocatalysis laboratory College of Materials Science and EngineeringQingdao University of Science and TechnologyQingdao266042PR China

Water splitting is an effective strategy to produce renewable and sustainable hydrogen ***,seawater splitting,avoiding use of the limited freshwater resource,is more ***,electrocatalysts explored for hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)using natural seawater or saline electrolyte have been increasingly *** better understand the current status and challenges of the electrocatalysts for HER and OER from seawater,we comprehensively review the recent advances in electro-catalysts for seawater *** fundamentals,challenges and possible strategies for seawater splitting are firstly ***,the recently reported electrocatalysts that explored for HER and OER from seawater are summarized and ***,the perspectives in the development of high-efficient electrocatalysts for seawater splitting are also proposed.

关键词： Seawater splitting Electrocatalysts Hydrogen evolution reaction Oxygen evolution reaction

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Filling the in situ-generated vacancies with metal cations captured by C-N bonds of defect-rich 3D carbon nanosheet for bifunctional oxygen electrocatalysis

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Journal of Energy Chemistry 2021年第8期30卷 47-54,I0002页

作者： Dawei Chen Wei Cao Jing Liu Jie Wang Xiaoke Li Luhua Jiang nanomaterial&electrocatalysis laboratory College of Materials Science and EngineeringQingdao University of Science and TechnologyQingdao 266042China

Nitrogen-doped carbon materials with vacancies/defects have been developed as highly efficient ORR electrocatalysts but with poor activity for OER,which limits their application in rechargeable metal-air *** the vacancies/defects with heteroatoms is expected to be an effective strategy to obtain surprising catalytic activities and improve their stability especially under the strongly oxidizing conditions during the OER ***,we successfully transformed the defect-rich 3 D carbon nanosheets(DCN)into a bifunctional ORR/OER electrocatalyst(DCN-M)by utilizing the in-situ generated vacancies to capture metal cations via a modified salt-sealed *** varying the metal(Fe,Ni)content,the captured metal cations in DCN-M existed in different chemical states,i.e.,metal atoms were stabilized by CàN bonds at low metal contents,while at high metal contents,bimetal particles were covered by graphene layers,taking responsibility for catalyzing the ORR and OER,*** addition,the in-situ formed graphene layers with an interconnected structure facilitate the electron transport during the *** Janus-feature of DCN-M in structures ensures superior bifunctional activity and good stability towards ORR/OER for the rechargeable Zn-air *** work provides an effective strategy to design multifunctional electrocatalysts by heteroatom filling into vacancies of carbon materials.

关键词： Carbon catalyst Vacancies/Defects Heteroatom filling Bifunctional oxygen electrocatalysis Rechargeable Zn-air battery

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Organic interfacial engineering of gold nanowires for selective glycerol electrooxidation

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Chinese Chemical Letters 2024年第3期35卷 502-507页

作者： Zhe Wang Qingling Hong Boqiang Miao Tianjiao Wang Yu Ding Pujun Jin Pei Chen Yu Chen Key laboratory of Macromolecular Science of Shaanxi Province Key Laboratory of Applied Surface and Colloid Chemistry(Ministry of Education)Shaanxi Key Laboratory for Advanced Energy DevicesSchool of Materials Science and EngineeringShaanxi Normal UniversityXi'an 710062China

The selective electrochemical conversion of glycerol into value-added products is a green and sustainable strategy for the biomass *** this work,Au nanowires(Au-NW)modified with polyethyleneimine(PEI)molecule(Au-NW@PEI)is obtained by an up-bottom post-modification *** characterization,molecular dynamics simulation and density functional theory demonstrate that the loose-packed PEI monolayer firmly and uniformly distribute on the Au-NW surface due to the strong Au-N *** experiments and product analysis display that PEI modification significantly enhance the electro-activity of Au-NW for the glycerol electro-oxidation reaction(GEOR)due to the electronic ***,the steric hindrance and electrostatic effect of PEI layer make the optimizing adsorption of intermediates ***,the selectivity of C3 product glyceric acid over Au-NW@PEI is increased by nearly 20%.The work thus indicates that the rational design of metal-organic interface can effectively elevate the electro-activity and selectivity of Au nanostructures,which may have wide application in biomass development.

关键词： Glycerol electrooxidation reaction Organic interface engineering Gold-based nanomaterials electrocatalysis Selectivity

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Unraveling role of double-exchange interaction in electrochemical water oxidation by external magnetic field

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Rare Metals 2024年第1期43卷 289-297页

作者： Jun Li Jun-Ming Li Hong Hong Dong-Xue Liu Qing-Qi Cao Dun-Hui Wang National laboratory of Solid State Microstructures and Jiangsu Provincial Key laboratory for Nanotechnology Nanjing UniversityNanjing 210093China School of Electronics and Information Hangzhou Dianzi UniversityHangzhou 310018China

Double-exchange(DE) interaction plays an important role in electrocatalytic oxygen evolution reaction(OER).However,precise achievement of DE interaction often requires foreign dopants or vacancy engineering,leading to destabilization of the catalysts and deterioration of *** contrast,the utilization of environmentally friendly,contactless,and continuously adjustable magnetic fields to study the OER process is profitable to avoid aforementioned interference factors and further elucidate the direct relationship_(0.5)between DE interaction and OER ***,by using cobalt hydroxide carbonate(Co(OH)(CO_(3))·xH_(2)O,CoHC) nanostructures as a proof-of-concept study,external magnetic fields are carefully implemented to verify the role of DE interaction during water oxidation *** studies reveal that external magnetic fields effectively enhance the reaction rate of the catalyst,the overpotential decreases from 386 to 355 mV(100 mA·cm^(-2)),while Tafel slopes drastically decline from 93 to 67 mV·dec^(-1)(1.0 T).Moreover,magnetic field increment exhibits robust *** in situ Raman and impedance measurements under external field,it can be found that magnetic field promotes the electron migration between Co^(2+) and Co^(3+) in the CoHC catalysts with the assistance of DE interactions,thus boosting the OER efficiency.

关键词： Magnetic field Double-exchange(DE)interaction electrocatalysis Oxygen evolution reaction(OER) Cobalt hydroxide carbonate

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Inducing mitochondriopathy-like damages by transformable nucleopeptide nanoparticles for targeted therapy of bladder cancer

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National Science Review 2024年第4期11卷 216-227页

作者： Da-Yong Hou Ni-Yuan Zhang Lu Wang Mei-Yu Lv Xiang-Peng Li Peng Zhang Yue-Ze Wang Lei Shen Xiu-Hai Wu Bo Fu Peng-Yu Guo Zi-Qi Wang Dong-Bing Cheng Hao Wang Wanhai Xu NHC and CAMS Key laboratory of Molecular Probe and Targeted Theranostics Heilongjiang Key Laboratory of Scientific Research in Urology Harbin Medical University Department of Urology Harbin Medical University Cancer Hospital CAS Key laboratory for Biomedical Effects of nanomaterials and Nanosafety CAS Center for Excellence in NanoscienceNational Center for Nanoscience and Technology(NCNST) School of Chemistry Chemical Engineering & Life Science Hubei Key Laboratory of Nanomedicine for Neurodegenerative Diseases Wuhan University of Technology

Mitochondriopathy inspired adenosine triphosphate(ATP) depletions have been recognized as a powerful way for controlling tumor growth. Nevertheless, selective sequestration or exhaustion of ATP under complex biological environments remains a prodigious challenge. Harnessing the advantages of in vivo self-assembled nanomaterials, we designed an Intracellular ATP Sequestration(IAS) system to specifically construct nanofibrous nanostructures on the surface of tumor nuclei with exposed ATP binding sites,leading to highly efficient suppression of bladder cancer by induction of mitochondriopathy-like ***, the reported transformable nucleopeptide(NLS-FF-T) self-assembled into nuclear-targeted nanoparticles with ATP binding sites encapsulated inside under aqueous conditions. By interaction with KPNA2, the NLS-FF-T transformed into a nanofibrous-based ATP trapper on the surface of tumor nuclei,which prevented the production of intracellular energy. As a result, multiple bladder tumor cell lines(T24,EJ and RT-112) revealed that the half-maximal inhibitory concentration(IC50) of NLS-FF-T was reduced by approximately 4-fold when compared to NLS-T. Following intravenous administration, NLS-FF-T was found to be dose-dependently accumulated at the tumor site of T24 xenograft mice. More significantly, this IAS system exhibited an extremely antitumor efficacy according to the deterioration of T24 tumors and simultaneously prolonged the overall survival of T24 orthotopic xenograft mice. Together, our findings clearly demonstrated the therapeutic advantages of intracellular ATP sequestration-induced mitochondriopathy-like damages, which provides a potential treatment strategy for malignancies.

关键词： self-assembly nucleopeptide nanomaterial bladder cancer mitochondriopathy

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Porous metal oxides in the role of electrochemical CO_(2) reduction reaction

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Journal of Energy Chemistry 2024年第1期88卷 373-398,I0009页

作者： Ziqi Zhang Jinyun Xu Yu Zhang Liping Zhao Ming Li Guoqiang Zhong Di Zhao Minjing Li Xudong Hu Wenju Zhu Chunming Zheng Xiaohong Sun School of Chemical Engineering and Technology Tianjin Key Laboratory of Green Chemical Technology and Process EngineeringState Key Laboratory of Separation Membrane and Membrane ProcessesTiangong UniversityTianjin 300387China School of Materials Science and Engineering Key Laboratory of Advanced Ceramics and Machining TechnologyMinistry of EducationTianjin UniversityTianjin 300072China

The global energy-related CO_(2) emissions have rapidly increased as the world economy heavily relied on fossil *** paper explores the pressing challenge of CO_(2) emissions and highlights the role of porous metal oxide materials in the electrocatalytic reduction of CO_(2)(CO_(2)RR).The focus is on the development of robust and selective catalysts,particularly metal and metal-oxide-based *** metal oxides offer high surface area,enhancing the accessibility to active sites and improving reaction *** tunability of these materials allows for tailored catalytic behavior,targeting optimized reaction mechanisms for CO_(2)*** work also discusses the various synthesis strategies and identifies key structural and compositional features,addressing challenges like high overpotential,poor selectivity,and low *** on these insights,we suggest avenues for future research on porous metal oxide materials for electrochemical CO_(2) reduction.

关键词： CO_(2)reduction Carbon dioxide Transformation Porous metal oxides electrocatalysis

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Recent advances in morphology control of platinum catalysts toward oxygen reduction reaction

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Frontiers in Energy 2024年第3期18卷 330-355页

作者： Shun CHEN Yanru LIU Xiaogang FU Wanglei WANG State Key laboratory of Solidification Processing Atomic Control and Catalysis Engineering LaboratorySchool of Materials Science and EngineeringNorthwestern Polytechnical UniversityXi’an 710072China State Key laboratory of Oral and Maxillofacial Reconstruction and Regeneration National Clinical Research Center for Oral DiseasesShaanxi Key Laboratory of StomatologyDepartment of Dental MaterialsSchool of StomatologyThe Fourth Military Medical UniversityXi’an 710032China

Exploring advanced platinum (Pt)-based electrocatalysts is vital for the widespread implementation of proton exchange membrane fuel cells (PEMFCs). Morphology control represents an effective strategy to optimize the behavior of Pt catalysts. In this work, an attempt is made to comprehensively review the effect of morphology control on the catalytic behavior of catalysts in the oxygen reduction reaction (ORR). First, the fundamental physicochemical changes behind morphology control, including exposing more active sites, generating appropriate lattice strains, and forming different crystalline surfaces, are highlighted. Then, recently developed strategies for tuning the morphologies of electrocatalysts, including core-shell structures, hollow structures, nanocages, nanowires, and nanosheets, are comprehensively summarized. Finally, an outlook on the future development of morphology control of Pt catalysts is presented, including rational design strategies, advanced in situ characterization techniques, novel artificial intelligence, and mechanical learning. This work is intended to provide valuable insights into designing the morphology and technological innovation of efficient redox electrocatalysts in fuel cells.

关键词： morphology platinum catalysts electrocatalysis ORR PEMFC

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Engineering and dynamics of heterogeneous catalysts via metal single atoms as promoters/precursors

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Science China Chemistry 2024年第8期67卷 2547-2565页

作者： Jiwei Li Junli Xu Jingyun Yang Zitao Duan Zhun Zhang Haifeng Xiong State Key laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Innovation laboratory for Sciences and Technologies of Energy Materials of Fujian Province Xiamen 361102China

Metal single-atom catalysts(SACs) have emerged as a focal point of research, captivating the scientific community due to their distinctive electronic properties and unparalleled catalytic prowess in the realm of heterogeneous catalysis. However, their significance transcends their role as mere active sites. Recent investigations have illuminated the multifaceted capabilities of metal single atoms as catalyst promoters and precursors, paving the way for the engineering of highly efficient heterogeneous catalysts. Single-atom promoters not only enhance the stabilization of active metals and tailor the support material, but regulate the reactive interfacial structure, eventually tuning the catalytic performance. Furthermore, SACs were also used as catalyst precursors to design new catalyst active sites. During the pretreatment or catalytic reaction, the structure of the metal single sites is changed significantly and transformed into the new and more active state, which improve the adsorption and reactive ability of reactants or intermediates. In this critical review, we comment the recent development of metal SACs used as catalyst promoters/precursors in engineering heterogeneous catalysts, including thermal catalysis and electrocatalysis. Furthermore, the dynamic evolution of the SACs during the pretreatment or catalytic reaction is also discussed. Finally, we provide our insight to potentially guide the future development on this emerging field.

关键词： single-atom catalysts single-atom promoter single-atom precursor dynamic evolution

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Enhanced hydrogen evolution reaction in FePt film with remanence due to decrease in domain walls

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Rare Metals 2024年第3期43卷 1108-1115页

作者： Hong Hong Dong-Xue Liu Jun Li Jun-Ming Li Li-Qian Wu Bo Yang Qing-Qi Cao Dun-Hui Wang National laboratory of Solid State Microstructures Collaborative Innovation Center of Advanced MicrostructuresJiangsu Provincial Key Laboratory for NanotechnologySchool of PhysicsNanjing UniversityNanjing210093China Hangzhou Dianzi University Hangzhou310018China Key laboratory for Anisotropy and Texture of Materials(Ministry of Education) School of Material Science and EngineeringNortheastern UniversityShenyang110819China

As an effective strategy to improve the properties of electrocatalysts,magnetic field-assisted electrocatalytic water splitting has attracted increasing attention ***,the corresponding enhancements mostly depend on the exertion of an external magnetic field during electrochemical reactions,which results in a high cost of industrial production,and makes the magnetic field manipulation of electrocatalysis become a challenging *** this work,instead of the external magnetic field,a bias magnetic field is self-supplied by the remanence state of a ferromagnetic electrocatalyst of *** to the assistance of this bias magnetic field,the FePt film in the remanence state shows the overpotential of 229 mV during hydrogen evolution reaction,which is much lower than that in its demagnetization state(283 mV).Our findings demonstrate that the remanence in ferromagnetic electrocatalysts can improve the catalytic performance,which is attributed to the decrease in domain walls.

关键词： Remanence Magnetic domains electrocatalysis Hydrogen evolution reaction(HER)

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