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Engineering hierarchical quaternary superstructure of an integrated MOF-derived electrode for boosting urea electrooxidation assisted water electrolysis

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Green Energy & Environment 2024年第4期9卷 695-701页

作者： Jianjun Tian Changsheng Cao Yingchun He Muhammad Imran Khan Xin-Tao Wu Qi-Long Zhu State Key laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of Sciences(CAS)Fuzhou350002China Fujian Science&Technology Innovation laboratory for Optoelectronic Information of China Fuzhou350108China University of Chinese Academy of Sciences Beijing100049China Research Institute of Sciences and Engineering(RISE) University of SharjahSharjah27272United Arab Emirates

Controllable design of the catalytic electrodes with hierarchical superstructures is expected to improve their electrochemical ***,a self-supported integrated electrode(NiCo-ZLDH/NF)with a unique hierarchical quaternary superstructure was fabricated through a self-sacrificing template strategy from the metal–organic framework(Co-ZIF-67)nanoplate arrays,which features an intriguing well-defined hierarchy when taking the unit cells of the NiCo-based layered double hydroxide(NiCo-LDH)as the primary structure,the ultrathin LDH nanoneedles as the secondary structure,the mesoscale hollow plates of the LDH nanoneedle arrays as the tertiary structure,and the macroscale three-dimensional frames of the plate arrays as the quaternary ***,the distinctive structure of NiCo-ZLDH/NF can not only accelerate both mass and charge transfer,but also expose plentiful accessible active sites with high intrinsic activity,endowing it with an excellent electrochemical performance for urea oxidation reaction(UOR).Specially,it only required the low potentials of 1.335,1.368 and 1.388 V to deliver the current densities of 10,100 and 200 mA cm^(-2),respectively,much superior to those for typical *** NiCo-ZLDH/NF as the bifunctional electrode for both anodic UOR and cathodic HER,an energy-saving electrolysis system was further explored which can greatly reduce the needed voltage of 213 mV to deliver the current density of 100 mA cm^(-2),as compared to the conventional water electrolysis system composed of *** work manifests that it is prospective to explore the hierarchically nanostructured electrodes and the innovative electrolytic technologies for high-efficiency electrocatalysis.

关键词： Hierarchical superstructures Metal–organic frameworks Layered double hydroxides Urea oxidation reaction Hydrogen evolution reaction

Quantum Spin Exchange Interactions to Accelerate the Redox Kinetics in Li–S Batteries

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Nano-Micro Letters 2024年第5期16卷 370-383页

作者： Yu Du Weijie Chen Yu Wang Yue Yu Kai Guo Gan Qu Jianan Zhang Key laboratory of Advanced Energy Catalytic and Functional Materials Preparation of Zhengzhou City College of Materials Science and EngineeringZhengzhou UniversityZhengzhou 450001People’s Republic of China

Spin-engineering with electrocatalysts have been exploited to suppress the“shuttle effect”in Li–S *** selec-tion,spin-dependent electron mobility and spin potentials in activation barriers can be optimized as quantum spin exchange interactions lead-ing to a significant reduction of the electronic repulsions in the orbitals of ***,we anchor the MgPc molecules on fluorinated carbon nanotubes(MgPc@FCNT),which exhibits the single active Mg sites with axial *** to the density functional theory calculations,the electronic spin polarization in MgPc@FCNT not only increases the adsorption energy toward LiPSs intermediates but also facilitates the tunneling process of electron in Li–S *** a result,the MgPc@FCNT provides an initial capacity of 6.1 mAh cm^(-2) even when the high sulfur loading is 4.5 mg cm^(-2),and still maintains 5.1 mAh cm^(-2) after 100 *** work provides a new perspective to extend the main group single-atom catalysts enabling high-performance Li–S batteries.

关键词： Metal phthalocyanines Spin polarization electrocatalysis Li–S batteries

Recent Advances in Mechanistic Understanding of Metal-Free Carbon Thermocatalysis and electrocatalysis with Model Molecules

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Nano-Micro Letters 2024年第7期16卷 74-97页

作者： Wei Guo Linhui Yu Ling Tang Yan Wan Yangming Lin CAS Key laboratory of Design and Assembly of Functional Nanostructures Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002People’s Republic of China Xiamen Key laboratory of Rare Earth Photoelectric Functional Materials Xiamen Institute of Rare Earth MaterialsHaixi InstituteChinese Academy of SciencesXiamen 361021People’s Republic of China State Key laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002People’s Republic of China Institute of Urban Environment Chinese Academy of SciencesXiamen 361021People’s Republic of China

Metal-free carbon,as the most representative heterogeneous metal-free catalysts,have received considerable interests in electro-and thermo-catalytic reac-tions due to their impressive performance and *** the past decade,well-designed carbon catalysts with tunable structures and heteroatom groups coupled with various characterization techniques have proposed numerous reaction ***,active sites,key intermediate species,precise structure-activity relationships and dynamic evolution processes of carbon catalysts are still rife with controversies due to the monotony and limitation of used experimental *** this Review,we sum-marize the extensive efforts on model catalysts since the 2000s,particularly in the past decade,to overcome the influences of material and structure limitations in metal-free carbon *** both nanomolecule model and bulk model,the real contribution of each alien species,defect and edge configuration to a series of fundamentally important reactions,such as thermocatalytic reactions,electrocatalytic reactions,were systematically *** with in situ techniques,isotope labeling and size control,the detailed reaction mechanisms,the precise 2D structure-activity relationships and the rate-determining steps were revealed at a molecular ***,the outlook of model carbon catalysis has also been proposed in this work.

关键词： Metal-free carbon catalysts Model catalyst electrocatalysis Active site Reaction mechanisms

In-situ transformed Mott-Schottky heterointerface in silver/manganese oxide nanorods boosting oxygen reduction,oxygen evolution,and hydrogen evolution reactions

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Nano Research 2024年第5期17卷 3622-3632页

作者： Ruiqi Cheng Kaiqi Li Huanxin Li Fengzhan Sun Xiaoqian He Tianshuo Zhao Jiao Zhang Chaopeng Fu Shanghai Key laboratory of Advanced High-temperature Materials and Precision Forming School of Materials Science and EngineeringShanghai Jiao Tong UniversityShanghai 200240China Christopher Ingold laboratory Department of ChemistryUniversity College LondonLondon WC1H 0AJUK Department of Chemistry Physical&Theoretical Chemistry LaboratoryUniversity of OxfordSouth Parks RoadOxford OX13QZUK Center of Hydrogen Science School of Materials Science and EngineeringShanghai Jiao Tong UniversityShanghai 200240China

The development of non-platinum group metal(non-PGM)and efficient multifunctional electrocatalysts for oxygen reduction reaction(ORR),oxygen evolution reaction(OER),and hydrogen evolution reaction(HER)with high activity and stability remains a great ***,by in-situ transforming silver manganese composite oxide heterointerface into boosted Mott-Schottky heterointerface through a facile carbon reduction strategy,a nanorod-like silver/manganese oxide with superior multifunctional catalytic activities for ORR,OER and HER and stability was *** nanorod-like silver/manganese oxide with Mott-Schottky heterointerface(designated as Ag/Mn_(3)O_(4))exhibits an ORR half-wave potential of 0.831 V(***)in 0.1 M KOH,an OER overpotential of 338 mV and a HER overpotential of 177 mV at the current density of 10 mA·cm^(-2)in 1 M KOH,contributing to its noble-metal benchmarks comparable performance in aqueous aluminum-air(Al-air)battery and laboratorial overall water splitting electrolytic ***,in-situ electrochemical Raman and synchrotron radiation spectroscopic measurements were conducted to further illustrate the catalytic mechanism of Ag/Mn_(3)O_(4)Mott-Schottky heterointerface towards various electrocatalytic *** the heterointerface,the Ag phase serves as the electron donor and the active phase for ORR and HER,while the Mn_(3)O_(4)phase serves as the electron acceptor and the active phase for OER,*** work deepens the understanding of the Mott-Schottky effect on electrocatalysis and fills in the gap in fundamental physical principles that are behind measured electrocatalytic activity,which offers substantial implications for the rational design of cost-effective multifunctional electrocatalysts with Mott-Schottky effect.

关键词： heterointerface electron donor-acceptor pair electrocatalyst Al-air battery water splitting

A novel responsive stabilizing Janus nanosilica as a nanoplugging agent in water-based drilling fluids for exploiting hostile shale environments

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Petroleum Science 2024年第2期21卷 1190-1210页

作者： Alain Pierre Tchameni Lv-Yan Zhuo Lesly Dasilva Wandji Djouonkep Robert Dery Nagre Lu-Xin Chen Lin Zhao Chao Ma Bin-Qiang Xie College of Petroleum Engineering Yangtze UniversityWuhan430100HubeiChina Key laboratory of Drilling and Production Engineering for Oil and Gas HubeiChina Lost Circulation Control laboratory National Engineering Laboratory for Petroleum Drilling EngineeringYangtze UniversityWuhan430100HubeiChina College of Petroleum Engineering Shandong Institute of Petroleum and Chemical TechnologyDongying257061ShandongChina Petroleum Engineer Research Institute of Petrochina Dagang Oilfield Tianjin300280China Department of Chemical Engineering Kumasi Technical UniversityP.O.Box 854KumasiGhana

Thermo-responsive nanocomposites have recently emerged as potential nanoplugging agents for shale stabilization in high-temperature water-based drilling fluids(WBDFs). However, their inhibitory properties have not been very effective in high-temperature drilling operations. Thermo-responsive Janus nanocomposites are expected to strongly interact with clay particles from the inward hemisphere of nanomaterials, which drive the establishment of a tighter hydrophobic membrane over the shale surface at the outward hemisphere under geothermal conditions for shale stabilization. This work combines the synergistic benefits of thermo-responsive and zwitterionic nanomaterials to synchronously enhance the chemical inhibitions and plugging performances in shale under harsh conditions. A novel thermoresponsive Janus nanosilica(TRJS) exhibiting zwitterionic character was synthesized, characterized,and assessed as shale stabilizer for WBDFs at high temperatures. Compared to pristine nanosilica(Si NP)and symmetrical thermo-responsive nanosilica(TRS), TRJS exhibited anti-polyelectrolyte behaviour, in which electrolyte ions screened the electrostatic attraction between the charged particles, potentially stabilizing nanomaterial in hostile shaly environments(i.e., up to saturated brine or API brine). Macroscopically, TRJS exhibited higher chemical inhibition than Si NP and TRS in brine, prompting a better capability to control pressure penetration. TRJS adsorbed onto the clay surface via chemisorption and hydrogen bonding, and the interactions became substantial in brine, according to the results of electrophoretic mobility, surface wettability, and X-ray diffraction. Thus, contributing to the firm trapping of TRJS into the nanopore structure of the shale, triggering the formation of a tight hydrophobic membrane over the shale surface from the outward hemisphere. The addition of TRJS into WBDF had no deleterious effect on fluid properties after hot-treatment at 190℃, implying that TRJ

关键词： Janus nanosilica Thermo-responsive copolymer Anti-polyelectrolyte effect Shale stabilizer Inhibition Plugging Drilling fluid

Surface iodine and pyrenyl-graphdiyne co-modified Bi catalysts for highly efficient CO_(2) electroreduction in acidic electrolyte

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Nano Research 2024年第4期17卷 2381-2387页

作者： Min Zhang Juan Wang Xin Rong Xiu-Li Lu Tong-Bu Lu MOE International Joint laboratory of Materials Microstructure Institute for New Energy Materials and Low Carbon TechnologiesSchool of Materials Science and EngineeringTianjin University of TechnologyTianjin 300384China

CO_(2) electroreduction to formic acid/formate would contribute to alleviating the energy and climate *** work reports a Bi-based catalyst derived from the in-situ electroreduction of Bi_(2)O_(2)CO_(3) modified with iodine and pyrenyl-graphdiyne(PGDY)on the surface for efficient electroreduction of CO_(2) in acidic electrolyte,with a high partial current density of 98.71 mA·cm^(-2) and high Faradaic efficiency(FE)>90%over the potential range from^(-1).2 to-1.5 V *** hydrogen electrode(RHE),as well as the long-term operational stability over 240 h without degradation in H-type *** results and density function theory calculations show that the synergistic effect of surface iodine and PGDY is responsible for this active and extremely stable process of CO_(2) electroreduction via lowering the energy barriers for formation of*OCHO intermediate,suppressing the competitive HER by enhancing the concentration of both K+and CO_(2) at reaction interface,as well as preventing the dissolution and re-deposition of active Bi atoms on surface during catalytic *** work provides new insight into designing highly active and stable electrocatalysts for CO_(2) reduction.

关键词： CO_(2) reduction electrocatalysis Bi-based catalysts acidic electrolyte

A Review on nanomaterial-based Strategies for Manipulating Tumor Microenvironment to Enhance Chemodynamic Therapy

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Chemical Research in Chinese Universities 2024年第2期40卷 202-212页

作者： CAO Mengyu XING Xiner SHEN Xiaotong OUYANG Jin NA Na Key laboratory of Radiopharmaceuticals Ministry of EducationCollege of ChemistryBeijing Normal UniversityBeijing100875P.R.China Department of Chemistry College of Arts and SciencesBeijing Normal University at ZhuhaiZhuhai519087P.R.China State Key laboratory of Biogeology and Environmental Geology China University of GeosciencesWuhan430074P.R.China

Cancer is a leading cause of death worldwide,and a series of strategies has been reported for tumor-specific ***,chemodynamic therapy(CDT)has become a research hotspot for antitumor treatment due to its advantages of high specificity,endogenous stimulation,and high ***,the therapeutic effects of CDT are normally limited in the complex tumor microenvironment(TME),such as insufficient acidity,tumor hypoxia,low hydrogen peroxide(H2O2),and high glutathione(GSH).Consequently,different kinds of multifunctional nanomaterials have been designed to manipulate TME conditions,which provided more opportunities to improve the efficiency of *** review focuses on nanomaterial-based strategies for enhancing CDT through manipulating *** CDT enhancements,this review would provide a reference for the future development of efficient CDT nanomaterials.

关键词： Chemodynamic therapy Tumor microenvironment nanomaterial Manipulating strategy Fenton/Fenton-like reaction

Making the Complicated Simple:A Minimizing Carrier Strategy on Innovative Nanopesticides

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Nano-Micro Letters 2024年第10期16卷 31-46页

作者： Wenjie Shangguan Qiliang Huang Huiping Chen Yingying Zheng Pengyue Zhao Chong Cao Manli Yu Yongsong Cao Lidong Cao State Key laboratory for Biology of Plant Diseases and Insect Pests Institute of Plant ProtectionChinese Academy of Agricultural SciencesBeijing 100193People's Republic of China College of Plant Protection China Agricultural UniversityBeijing 100193People's Republic of China State Key laboratory of Element-Organic Chemistry Department of Chemical BiologyCollege of ChemistryNankai UniversityTianjin 300071People's Republic of China

The flourishing progress in nanotechnology offers boundless opportunities for agriculture,particularly in the realm of nanopesticides research and ***,concerns have been raised regarding the human and environmental safety issues stemming from the unrestrained use of non-therapeutic nanomaterials in *** is also important to consider whether the current development strategy of nanopesticides based on nanocarriers can strike a balance between investment and return,and if the complex material composition genuinely improves the efficiency,safety,and circularity of ***,we introduced the concept of nanopesticides with minimizing carriers(NMC)prepared through prodrug design and molecular self-assembly emerging as practical tools to address the current limitations,and compared it with nanopesticides employing non-therapeutic nanomaterials as carriers(NNC).We further summarized the current development strategy of NMC and examined potential challenges in its preparation,performance,and ***,we asserted that the development of NMC systems can serve as the innovative driving force catalyzing a green and efficient revolution in nanopesticides,offering a way out of the current predicament.

关键词： Nanopesticides Green agrochemicals Self-assembly nanomaterial safety Sustainable development strategies

How the surface Cu layer affected the activity of Ni foil for alkaline hydrogen evolution

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Journal of Materials Science & Technology 2024年第2期169卷 11-18页

作者： Qingfeng Hu Yuan Liu Xuerong Zheng Jinfeng Zhang Jiajun Wang Xiaopeng Han Yida Deng Wenbin Hu School of Materials Science and Engineering Key Laboratory of Advanced Ceramics and Machining Technology of Ministry of EducationTianjin UniversityTianjin 300072China State Key laboratory of Marine Resource Utilization in South China Sea School of Materials Science and EngineeringHainan UniversityHaikou 570228China Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityBinhai New CityFuzhou 350207China

Synthesizing bimetallic nanomaterials,with noble metals as the surface layers and inert metals as the substrates,has been proven to be an effective way to reduce the use of noble metals with maintained catalytic ***,an atomic diffusion from the inert substrate to the surface during the long-term operation has been reported to significantly decrease the *** this work,a series of catalysis-inert Cu-coated Ni foil were fabricated through electrodeposition and their activities for alkaline hydrogen evolution were ***,the Ni/Cu-60 sample showed a similar catalytic property with pure Ni foil and only a slight decrease in HER activity was *** X-ray photoelectron spectroscopy(XPS)results indicated a decreased electron concentration of Cu in Ni/Cu-60,and theoretical calculations further demonstrated the electron transfer between the Ni substrate and Cu *** results reveal that a specific composition or structure of an inert metal layer might not significantly decrease the electrocatalytic activity of active ***,there are more possibilities for the rational design of metal-based catalysts for electrocatalysis.

关键词： Bimetallic heterostructure Charge redistribution Water splitting Alkaline hydrogen evolution