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Enriched electrophilic oxygen species facilitate acidic oxygen evolution on Ru-Mo binary oxide catalysts

Nano Research 2024年第3期17卷 1165-1172页

作者： Yaya Wang Yunzhou Wen Yumeng Cheng Xinhong Chen Mengjiao Zhuansun Tongbao Wang Jun Li Debora Meira Huarui Sun Jun Wei Jia Zhou Yuhang Wang Sisi He Shenzhen Key Laboratory of Flexible Printed Electronics Technology Harbin Institute of Technology(Shenzhen)University TownShenzhen 518055China School of Science Harbin Institute of Technology(Shenzhen)University TownShenzhen 518055China Institute of Functional Nano&Soft Materials(FUNSOM) Jiangsu Key Laboratory of Advanced Negative Carbon TechnologiesSoochow UniversitySuzhou 215123China Frontiers Science Center for Transformative Molecules Shanghai Jiao Tong UniversityShanghai 200240China Science Division Canadian Light SourceSaskatoonSKS7N 2V3Canada Photon Science Division Argonne National LaboratoryLemontIL60439USA School of Materials Science and Engineering Harbin Institute of Technology(Shenzhen)University TownShenzhen 518055China

The polymer electrolyte membrane(PEM)electrolyzers are burdened with costly iridium(Ir)-based catalysts and high operation overpotentials for the oxygen evolution reaction(OER).The development of earth-abundant,highly active,and durable electrocatalysts to replace Ir is a critical step in reducing the cost of green hydrogen *** we develop a Ru5Mo4Ox binary oxide catalyst that exhibits high activity and stability in acidic *** electron-withdrawing property of Mo enriches the electrophilic surface oxygen species,which promotes acidic OER to proceed via the adsorbate evolution *** a result,we achieve a 189 mV overpotential at 10 mA·cm^(-2) and a Tafel slope of 48.8 mV·dec^(-1).Our catalyst demonstrates a substantial 18-fold increase in intrinsic activity,as evaluated by turnover frequency,compared to commercially available RuO_(2) and IrO_(2) ***,we report a stable OER operation at 10 mA·cm^(-2) for 100 h with a low degradation rate of 2.05 mV·h^(-1).

关键词： electrocatalysis oxygen evolution reaction(OER) ruthenium(Ru)-based oxide molybdenum electrophilic oxygen

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Heterophase junction engineering-induced Co spin-state modulation of CoSe_(2) for large-current hydrogen evolution reaction

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Rare Metals 2024年第6期43卷 2660-2670页

作者： Bao-Chai Xu Ya-Ping Miao Min-Qin Mao Dong-Lian Li Song Xie Wei-Hong Jin Shu Xiao Jing Wen Zaenab Abd-Allah Zhi-Tian Liu Xiang Peng Paul K.Chu Hubei Key Laboratory of Plasma Chemistry and Advanced Materials School of Materials Science and EngineeringWuhan Institute of TechnologyWuhan 430205China School of Textile Science and Engineering Xi'an Polytechnic UniversityXi'an 710048China Institute of Advanced Wear and Corrosion Resistant and Functional Materials Jinan UniversityGuangzhou 510632China Institute of Safety Science and Engineering South China University of TechnologyGuangzhou 510641China Department of Engineering Manchester Metropolitan UniversityManchester M156BHUK Department of Physics Department of Materials Science and Engineeringand Department of Biomedical EngineeringCity University of Hong KongHong Kong 999077China

Efficient electrocatalysts are vital to large-current hydrogen production in commercial water splitting for green energy ***,a novel heterophase engineering strategy is described to produce polymorphic CoSe_(2)*** composition of the electrocatalysts consisting of both cubic CoSe_(2)(c-CoSe_(2))and orthorhombic CoSe_(2)(o-CoSe_(2))phases can be controlled *** results demonstrate that junction-induced spin-state modulation of Co atoms enhances the adsorption of intermediates and accelerates charge transfer resulting in superior large-current hydrogen evolution reaction(HER)***,the CoSe_(2)based heterophase catalyst with the optimal c-CoSe_(2)content requires an overpotential of merely 240 mV to achieve 1,000 mA·cm^(-2)as well as a Tafel slope of 50.4 mV·dec^(-1).Furthermore,the electrocatalyst can maintain a large current density of 1,500 mA·cm^(-2)for over 320 h without *** results reveal the advantages and potential of heterophase junction engineering pertaining to design and fabrication of low-cost transition metal catalysts for large-current water splitting.

关键词： Heterophase junction Spin-state Hydrogen evolution reaction Large current electrochemical hydrogen production Water splitting

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Synthesis of Three-Dimensional Chiral Covalent Organic Frameworks Using Surfactant as Inducer in Water

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Chinese Journal of Chemistry 2024年第23期42卷 3093-3098页

作者： Meiying Huang Zhipeng Zhou Xin Dong Yuyao Li Yonghang Yang Changye Zhan Jiaxing Lu Xiaoshu Wei Yuexian Hong Weiqi Cheng Wei Liu Zhongke Yuan Xudong Chen Zhikun Zheng Key Laboratory for Polymeric Composite and Functional Materials of Ministry of Education School of Chemistryand State Key Laboratory of Optoelectronic Materials and TechnologiesSun Yat-sen UniversityGuangzhouGuangdong 510275China College of Chemistry and Molecular Engineering Beijing National Laboratory for Molecular SciencesPeking UniversityBeijing 100871China Department of Stomatology Sun Yat-sen Memorial HospitalSun Yat-sen UniversityGuangzhouGuangdong 510275China Key Laboratory of Low-Carbon Chemistry and Energy Conservation of Guangdong Province Key Laboratory for Polymeric Composite and Functional Materials of Ministry of EducationSchool of Materials Science and Engineeringand State Key Laboratory of Optoelectronic Materials and TechnologiesSun Yat-sen UniversityGuangzhouGuangdong 510275China School of Chemical Engineering and Light Industry Guangdong University of TechnologyGuangzhouGuangdong 510006China Jieyang Branch of Chemistry and Chemical Engineering Guangdong Laboratory JieyangGuangdong 522031China

Chiral covalent organic frameworks(COFs)have shown promising applications in asymmetric catalysis,enantiomer separation and chiral recognition due to their tunable structures and permanent ***,synthesis of chiral COFs mainly relies on direct-synthesis method which requires asymmetric monomers to polymerize and crystallize with symmetric monomers and post-synthesis method which has been greatly limited to having complete reactions with the micro-/meso-sized pores of ***,the synthesis of two-dimensional COFs by covalent replacement of chiral competitor has been ***,we present the synthesis of three types of 3D COFs with tunable chirality using chiral amino acid derivative surfactant as inducer in water under ambient *** hydrogen bonds and electrostatic interactions between amino acid derivative surfactant and monomers as well as their precursors facilitate the transfer of the chirality.

关键词： Covalent organic frameworks Chirality Surfactants Amino acid derivatives Aqueous-phase synthesis Noncovalent interactions

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Highly crystalline core dominated the catalytic performance of carbon dot for cyclohexane to adipic acid reaction

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Nano Research 2022年第8期15卷 7662-7669页

作者： Xiao Wang Wenyi Bian Tianyang Zhang Yajie Zhao Mingwang Shao Haiping Lin Yang Liu Hui Huang Zhenhui Kang Institute of Functional Nano&Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials&DevicesSoochow UniversitySuzhou 215123China Macao Institute of Materials Science and Engineering(MIMSE) MUST-SUDA Joint Research Center for Advanced Functional MaterialsMacao University of Science and TechnologyTaipa 999078MacaoChina School of Physics and Information Technology Shaanxi Normal UniversityXi’an 710062China

Carbon dots(CDs)have uniquely structural,physicochemical and photochemical properties,suggesting a promising platform for catalysis *** in-depth understanding of the structure-activity relationship in the CDs-based catalyst system needs to know the effect of the crystalline core on their catalytic *** efficient catalytic oxidation of cyclohexane is an urgent challenge in current chemical industry,in which,adipic acid(AA)plays an important role in industry for synthesis of nylon6 and ***,we fabricated the pristine CDs by electrochemical etching graphite rod method and derived CDs with high crystalline core(CD-600,CD-800,and CD-1100)through a thermal treatment method in tube ***,these CDs performed an outstanding catalytic performance for one-step synthesis of AA from *** the help of machine learning(ML),the deep correlations between features(structures of CDs,catalytic conditions)and catalytic performances were investigated by XGBoost(XGB)*** under the optimization and prediction of XGB,it was found that high crystalline core preceded the other features and CD-1100 could get the best conversion of 30.696%and selectivity to AA of 92.52%at reaction conditions of 130℃,1.5 MPa,and 10 *** work pioneered the application of ML in industrial issues and demonstrated a comprehensive understanding on CDs as catalyst to realize one-step synthesis of AA.

关键词： adipic acid carbon dots machine learning catalytic performances crystalline core

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Anti-corrosion performance of Si-surface-alloying NdFeB magnets obtained with magnetron sputtering and thermal diffusion

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Journal of Rare Earths 2023年第8期41卷 1203-1210,I0003页

作者： Jin Tao Bang Liu Pengjie Zhang Guangqing Xu Jun Lv Jun Huang Jian Yan Wei Sun Bingshan Li Dongmei Wang Yucheng Wu School of Materials Science and Engineering Hefei University of TechnologyHefei 230009China BGRIMM Technology Group Co. Ltd.Beijing 102600China National Engineering Research Center for Magnetic Materials Beijing 102600China Key Laboratory of Advanced Functional Materials and Devices of Anhui Province Anhui Provincial International S&T Cooperation Base for Advanced Energy MaterialsHefei University of TechnologyHefei 230009China

Si alloying in the surface layer of NdFeB magnets was realized by thermal diffusion combined with magnetron *** surface composition,phase structure and morphology of NdFeB(S-Si)specimens were characterized by an X-ray diffractometer,an X-ray photoelectron spectrometer and a field emission scanning electron microscope,*** corrosion resistance of bare NdFeB(S-Si)was analyzed by static full immersion corrosion test and electrochemical *** of sputtering and thermal diffusion on the microstructure and corrosion resistance of the surface layer were *** show that surface alloying layer can effectively improve the corrosion resistance of bare NdFeB with the optimized static total immersion corrosion test time in NdFeB(1S-Si)-800 of 36 h,which is much longer than that of the pristine NdFeB(less than 0.5 h).The E_(corr)of NdFeB(1S-Si)-800 positively shifts from-1.05 to-0.92 V,indicating that the corrosion tendency is obviously *** J_(corr)is1.45×10^(-6)A/cm^(2)which is 2 orders of magnitude lower than that of the pristine NdFeB(5.25×10^(-4)A/cm^(2)).The intergranular composite oxides existing in Nd-rich phase contribute to the enhancement of corrosion resistance of Si-surface-alloying NdFeB.

关键词： NdFeB magnets Si surface alloying Magnetron sputtering Thermal diffusion Corrosion resistance Rare earths

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Selection of Negative Charged Acidic Polar Additives to Regulate Electric Double Layer for Stable Zinc Ion Battery

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Nano-Micro Letters 2024年第12期16卷 342-356页

作者： Xing Fan Lina Chen Yongjing Wang Xieyu Xu Xingxing Jiao Peng Zhou Yangyang Liu Zhongxiao Song Jiang Zhou State Key Laboratory for Mechanical Behavior of Materials Xi’an Jiaotong UniversityXi’an 710049People’s Republic of China School of Materials Science and Engineering Harbin Institute of Technology(Shenzhen)Shenzhen 518055People’s Republic of China Research Institute of Frontier Science Southwest Jiaotong UniversityChengdu 610031People’s Republic of China Hunan Provincial Key Defense Laboratory of High Temperature Wear-Resisting Materials and Preparation Technology Hunan University of Science and TechnologyXiangtan 411201People’s Republic of China School of Instrument Science and Technology Xi’an Jiaotong UniversityXi’an 710049People’s Republic of China School of Materials Science and Engineering Hunan Provincial Key Laboratory of Electronic Packaging and Advanced Functional MaterialsCentral South UniversityChangsha 410083People’s Republic of China

Zinc-ion batteries are promising for large-scale electrochemical energy storage systems,which still suffer from interfacial issues,e.g.,hydrogen evolution side reaction(HER),self-corrosion,and uncontrollable dendritic Zn *** the regulation of electric double layer(EDL)has been verified for interfacial issues,the principle to select the additive as the regulator is still ***,several typical amino acids with different characteristics were examined to reveal the interfacial behaviors in regulated EDL on the Zn *** charged acidic polarity(NCAP)has been unveiled as the guideline for selecting additive to reconstruct EDL with an inner zincophilic H_(2)O-poor layer and to replace H_(2)O molecules of hydrated Zn^(2+)with NCAP *** the synergistic effects of EDL regulation,the uncontrollable interface is significantly stabilized from the suppressed HER and anti-self-corrosion with uniform ***,by adding NCAP glutamate,a high average Coulombic efficiency of 99.83%of Zn metal is achieved in Zn|Cu asymmetrical cell for over 2000 cycles,and NH4V4O10|Zn full cell exhibits a high-capacity retention of 82.1%after 3000 cycles at 2 A g^(-1).Recapitulating,the NCAP principle posted here can quicken the design of trailblazing electrolyte additives for aqueous Zn-based electrochemical energy storage systems.

关键词： Aqueous Zn-ion batteries Zn metal anode Negative charged acidic polar additives Electric double-layer regulation

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Heavy-atom-free orthogonal configurative dye 1,7-di-anthra-aza-BODIPY for singlet oxygen generation

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Chinese Chemical Letters 2024年第10期35卷 291-294页

作者： Yan Zhu Jia Liu Meiheng Lv Tingting Wang Dongxiang Zhang Rong Shang Xin-Dong Jiang Jianjun Du Guiling Wang Liaoning&Shenyang Key Laboratory of Functional Dye and Pigment Shenyang University of Chemical TechnologyShenyang 110142China Department of Cell Biology China Medical UniversityShenyang 110122China State Key Laboratory of Fine Chemicals Dalian University of TechnologyDalian 116024China Department of Chemistry Graduate School of Advanced Science and EngineeringHiroshima UniversityHigashi-Hiroshima 7398526Japan

Spin-orbit,charge-transfer intersystem crossing(SOCT-ISC)can directly overcome the disadvantages of the traditional heavy-atom effect and improve the generation efficiency of reactive oxygen species(ROS).Since orthogonal molecular orbitals of donor-acceptor(D-A)pairs favor the SOCT-ISC transition,herein aza-borondipyrromethenes(aza-BODIPYs)with 1,7-di-anthracyl groups(An-azaBDP)was successfully prepared,owing to steric hindrance to produce a big dihedral angle between the two molecular orbital(MO)***,according to density functional theory(DFT)and time-dependent density functional theory(TDDFT),the energy difference between the S1-T1orbitals of An-aza BDP is small and more inclined towards ***-aza BDP can effectively generate singlet oxygen under light ***-aza BDP with light irradiation can induce apoptosis in SW620 cells,and can serve as a potential candidate for the treatment of cancer cells and tumors.

关键词： Orthogonal configuration Anthracene Heavy-atom-free Aza-BODIPY Singlet oxygen

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Atomic CoN_(3)S_(1) sites for boosting oxygen reduction reaction via an atomic exchange strategy

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Nano Research 2022年第3期15卷 1803-1808页

作者： Qianjun Zhi Rong Jiang Wenping Liu Tingting Sun Kang Wang Jianzhuang Jiang Beijing Advanced Innovation Center for Materials Genome Engineering Beijing Key Laboratory for Science and Application of Functional Molecular and Crystalline MaterialsDepartment of Chemistry and Chemical EngineeringSchool of Chemistry and Biological EngineeringUniversity of Science and Technology BeijingBeijing 100083China

It is vitally important to develop high-efficiency low-cost catalysts to boost oxygen reduction reaction(ORR)for renewable energy ***,an A-CoN_(3)S_(1)@C electrocatalyst with atomic CoN_(3)S_(1)active sites loaded on N,S-codoped porous carbon was produced by an atomic exchange *** constructed A-CoN_(3)S_(1)@C electrocatalyst exhibits an unexpected half-wave potential(0.901 V *** hydrogen electrode)with excellent durability for ORR under alkaline conditions(0.1 M KOH),superior to the commercial platinum carbon(20 wt.%Pt/C).The outstanding performance of A-CoN_(3)S_(1)@C in ORR is due to the positive effect of S atoms doping on optimizing the electron structure of the atomic CoN_(3)S_(1)active ***,the rechargeable zinc-air battery in which both A-CoN_(3)S_(1)@C and IrO_(2)were simultaneously served as cathode catalysts(A-CoN_(3)S_(1)@C&IrO_(2))exhibits higher energy efficiency,larger power density,as well as better stability,compared to the commercial Pt/C&IrO_(2)-based zinc-air *** present result should be helpful for developing lower cost and higher performance ORR catalysts which is expected to be used in practical applications in energy devices.

关键词： atomic sites oxygen reduction reaction CoN_(3)S_(1) zinc-air battery

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Blocking thermal runaway propagation in large-format sodium-ion battery system through localized energy release

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Journal of Energy Chemistry 2025年第5期104卷 514-526页

作者： Yongchun Dang Yongchao Yu Zhenpo Wang Peng Liu Xunli Zhou Yongjie Zhao Peipei Qi Fei Xu Lei Li National Engineering Research Center of Electric Vehicles Beijing Co-Innovation Centre for Electric VehiclesBeijing Institute of TechnologyBeijing 100081China Beijing Institute of Technology Chongqing Innovation Center Chongqing 401120China Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Applications School of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081China Research Center of Do-Fluoride New Energy Technology Co. Ltd.Jiaozuo 454003HenanChina

Cascading thermal runaway(TR)propagation poses a critical safety concern for large-format sodium-ion battery(SIB)systems because of the heightened risks of fires or ***,effectively suppressing TR propagation without introducing unintended side effects remains a significant ***,we demonstrate a localized energy release method to mitigate TR,by reducing the state of charge(SOC)of cells adjacent to the thermally runaway *** discover that as the SOCs decreased from 100%to 25%,the TR trigger temperature decreased significantly,and the maximum temperature decrease from 367 to 229℃.Meanwhile,the volume of gas decreased to one-third of its original value,while the range of explosion limits significantly *** analysis of the morphology of the debris further confirms that the structural damage is greater at higher SOC ***,an Entropy Weight and Technique for Order Preference by Similarity to an Ideal Solution(EW-TOPSIS)method has been established to assess the safety status of SIBs,showing that the TR possibility is nearly linear with the SOCs,and the TR hazard is exponentially related to the ***,when the SOC of cells adjacent to the TR cell is reduced to 25%,TR can be directly blocked without the need for additional cooling or thermal insulation *** study not only advances the understanding of TR behavior in SIBs but also offers a straightforward approach to mitigating the TR risk in SIB systems.

关键词： Sodium-ion battery Thermal runaway Safety assessment Localized energy release

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Recent advances in flexible self-oscillating actuators

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escience 2024年第5期4卷 91-109页

作者： Jingjing Li Wenjin Guo Weiqiang Zhao Yutian Zhu Jie Bai Zhigang Xia Xiang Zhou Zunfeng Liu School of Textile Science and Engineering State Key Laboratory of New Textile Materials and Advanced Processing TechnologiesWuhan Textile UniversityWuhan 430200China State Key Laboratory of Medicinal Chemical Biology Key Laboratory of Functional Polymer MaterialsTianjin Key Laboratory of Functional Polymer MaterialsSmart Sensing Interdisciplinary Science CenterCollege of ChemistryNankai UniversityTianjin 300350China College of Material Chemistry and Chemical EngineeringKey Laboratory of Organosilicon Chemistry and Material TechnologyMinistry of EducationKey Laboratory of Organosilicon Material TechnologyHangzhou Normal UniversityHangzhou 311121China College of Chemistry and Chemical Engineering Inner Mongolia Univ TechnolChem Engn CollHohhot 010051China Department of Science China Pharmaceutical UniversityNanjing 211198China

Soft actuators are constituted by a type of intelligent materials,and they can generate reversible mechanical motions under external *** usually achieve continuous actuation by manual turning on or off the power supply,which significantly increases the operation *** contrast,self-oscillating actuators can achieve autonomous motions under constant stimuli,and have recently attained great advancements,as well as promoted the development of autonomous soft *** this review,the latest achievements of soft oscillators are ***,the self-oscillating mechanisms mainly including oscillating chemical reactions and self-shadowing-induced mechanical negative feedback loops are *** oscillators constructed with various materials and configurations,driven by different stimuli and applied in different fields are then presented in ***,the difficulties and hopes of oscillators are ***,self-oscillating actuators are in the stage of vigorous development,and we believe that in the future,they will be used in various fields and make many scenarios more intelligent and autonomous.

关键词： Oscillating actuator Artificial muscles Polymer composite Biomimetic Smart materials

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