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In-situ study of the hydrogen peroxide photoproduction in seawater on carbon dot-based metal-free catalyst under operation condition

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Nano Research 2024年第7期17卷 5956-5964页

作者： Jiaxuan Wang Jiacheng Li Zenan Li Jie Wu Honglin Si Yangbo Wu Zhiyong Guo Xuepeng Wang Fan Liao Hui Huang Mingwang Shao Yang Liu Zhenhui Kang Institute of Functional Nano and Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials&DevicesSoochow UniversitySuzhou 215123China Faculty of Electrical Engineering and Computer Science Ningbo UniversityNingbo 315211China State Key Laboratory for Managing Biotic and Chemical Threats to the Quality and Safety of Agro-products School of Material Science and Chemical EngineeringNingbo UniversityNingbo 315211China Macao Institute of Materials Science and Engineering(MIMSE) MUST-SUDA Joint Research Center for Advanced Functional MaterialsMacao University of Science and TechnologyTaipa 999078MacaoChina

Hydrogen peroxide(H_(2)O_(2))photoproduction in seawater with metal-free photocatalysts derived from biomass materials is a green,sustainable,and ultra environmentally friendly ***,most photocatalysts are always corroded or poisoned in seawater,resulting in a significantly reduced catalytic ***,we report the metal-free photocatalysts(RUT-1 to RUT-5)with in-situ generated carbon dots(CDs)from biomass materials(Rutin)by a simple microwave-assisted pyrolysis *** visible light(λ≥420 nm,81.6 mW/cm^(2)),the optimized catalyst of RUT-4 is stable and can achieve a high H_(2)O_(2)yield of 330.36μmol/L in seawater,1.78 times higher than that in normal *** transient potential scanning(TPS)tests are developed and operated to in-situ study the H_(2)O_(2)photoproduction of RUT-4 under operation ***-4 has strong oxygen(O_(2))absorption capacity,and the O_(2)reduction rate in seawater is higher than that in *** cations in seawater further promote the photo-charge separation and facilitate the photo-reduction *** RUT-4,the conduction band level under operating conditions only satisfies the requirement of O_(2)reduction but not for hydrogen(H2)*** work provides new insights for the in-situ study of photocatalyst under operation condition,and gives a green and sustainable path for the H_(2)O_(2)photoproduction with metal-free catalysts in seawater.

关键词： carbon dots hydrogen peroxide photocatalysis transient potential scanning in-situ study operation condition

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Editorial for special issue on electromagnetic wave absorbing materials

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International Journal of Minerals,Metallurgy and materials 2023年第3期30卷 401-404页

作者： Guanglei Wu Hongjing Wu Zirui Jia Institute of Materials for Energy and Environment State Key Laboratory of Bio-fibers and Eco-textilesCollege of Materials Science and EngineeringQingdao UniversityQingdao 266071China MOE Key Laboratory of Material Physics and Chemistry under Extraordinary School of Physical Science and TechnologyNorthwestern Polytechnical UniversityXi’an 710072China College of Chemistry and Chemical Engineering Qingdao UniversityQingdao 266071China

With the rapid development of information technology and electronics industry,stealth warplanes,radar stealth,electronic countermeasures,microwave communications,and other equipment have played an increasingly important role in military ***,the design and development of new electromagnetic wave(EMW)absorbing materials with high performance and environmental applicability that can be widely used in the microwave field has become a key issue and a major strategic challenge that needs to be urgently addressed in the modernization and upgrading of major advanced military ***,how to effectively address the growing electromagnetic pollution has been an important issue that has plagued researchers in the field of EMW absorption for many years.

关键词： absorbing microwave wave

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Electric field controlled superlubricity of fullerene-based host–guest assembly

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Nano Research 2023年第1期16卷 583-588页

作者： Shanchao Tan Hongyu Shi Xin Du Kunpeng Wang Haijun Xu Junhua Wan Ke Deng Qingdao Zeng Yuhong Liu State Key Laboratory of Tribology Tsinghua UniversityBeijing 100084China CAS Key Laboratory of Standardization and Measurement for Nanotechnology CAS Center for Excellence in NanoscienceNational Center for Nanoscience and Technology(NCNST)Beijing 100190China College of Chemical Engineering Jiangsu Key Lab of Biomass-based Green Fuels and ChemicalsNanjing Forestry UniversityNanjing 210037China Key Laboratory of Organosilicon Chemistry and Material Technology of Ministry of Education Hangzhou Normal UniversityHangzhou 310012China Center of Materials Science and Optoelectonics Engineering University of Chinese Academy of SciencesBeijing 100049China

Controlling friction by the electric field is a promising way to improve the tribological performance of a variety of movable mechanical *** this work,the assembly structure and microscale superlubricity of a host–guest assembly are effectively controlled by the electric *** the help of the scanning tunneling microscopy(STM)technique,the host–guest assembly structures constructed by the co-assembly of fullerene derivative(Fluorene-C60)with macrocycles(4B2A and 3B2A)are explicitly *** with density functional theory(DFT),the distinct different assembly behaviors of fullerene derivatives are revealed at different probe biases,which is attributed to the molecular polarity of the fullerene *** the control on the adsorption behavior,the friction coefficient of host–guest assembly is demonstrated to be controllable in the electric field by using atomic force microscopy(AFM).At positive probe bias,the friction coefficient of the host–guest assembly is significantly reduced and achieves superlubricity(μmin=0.0049).The efforts not only help us gain insight into the host–guest assembly mechanism controlled by the electric field,but also promote the further application of fullerene in micro-electro-mechanical systems(MEMS).

关键词： superlubricity electric field friction control fullerene derivative host-guest assembly

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A Bifunctional Brønsted Acidic Deep Eutectic Solvent to Dissolve and Catalyze the Depolymerization of Alkali Lignin

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Journal of Renewable materials 2021年第2期9卷 219-235页

作者： Lifen Li Zhigang Wu Xuedong Xi Baoyu Liu Yan Cao Hailong Xu Yingcheng Hu College of Forestry Guizhou UniversityGuiyang550025China ENSTIB-LERMAB University of LorraineEpinal88051France Special and Key Laboratory for Development and Utilization of Guizhou Superior Bio-Based Materials Guizhou Minzu UniversityGuiyang550025China Key Laboratory of Bio-Based Material Science and Technology of Ministry of Education of China College of Material Science and EngineeringNortheast Forestry UniversityHarbin150040China

Lignin is an abundant renewable macromolecular material in nature,and degradation of lignin to improve its hydroxyl content is the key to its efficient *** lignin(AL)was treated with Brønsted acidic deep eutectic solvent(DES)based on choline chloride and p-toluenesulfonic acid at mild reaction temperature,the structure of the lignin before and after degradation,as well as the composition of small molecules of lignin were analyzed in order to investigate the chemical structure changes of lignin with DES treatment,and the degradation mechanism of lignin in this acidic DES was elucidated in this *** and NMR analyses demonstrated the selective cleavage of the lignin ether linkages in the degradation process,which was in line with the increased content of phenolic hydroxyl *** revealed that the O/C atomic ratio of the regenerated lignin was lower than that of the AL sample,revealing that the lignin underwent decarbonylation during the DES *** lignin with low molecular weight and narrow polydispersity index was obtained,and the average molecular weight(Mw)decreased from 17680 g/mol to 2792 g/mol(130°C,3 h)according to GPC *** lignin-degraded products were mainly G-type phenolics and ketones,and small number of aldehydes were also generated,the possible degradation pathway of lignin in this acidic DES was proposed.

关键词： Alkali lignin depolymerization Brønsted acidic deep eutectic solvent structural analysis

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Ambient Fast Synthesis of Superaerophobic/Superhydrophilic Electrode for Superior Electrocatalytic Water Oxidation

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Energy & Environmental materials 2023年第6期6卷 356-363页

作者： Jingjun Shen Jing Li Bo Li Yun Zheng Xiaozhi Bao Junpo Guo Yan Guo Chenglong Lai Wen Lei Shuangyin Wang Huaiyu Shao Guangdong-Hong Kong-Macao Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices Institute of Applied Physics and Materials EngineeringUniversity of MacaoAvenida da UniversidadeTaipaMacaoSAR 999078China Key Laboratory for Polymeric Composite and Functional Materials of Ministry of Education Key Laboratory of High Performance Polymer-based Composites of Guangdong ProvinceSchool of ChemistrySun Yat-Sen UniversityGuangzhou 510275China School of Materials Science and Engineering Huazhong University of Science and TechnologyWuhan 430074China The State Key Laboratory of Refractories and Metallurgy Wuhan University of Science and TechnologyWuhan 430081China State Key Laboratory of Chem/Bio-Sensing and Chemometrics Provincial Hunan Key Laboratory for Graphene Materials and DevicesCollege of Chemistry and Chemical EngineeringHunan UniversityChangsha 410082China

Developing cost-effective and facile methods to synthesize efficient and stable electrocatalysts for large-scale water splitting is highly desirable but remains a significant *** this study,a facile ambient temperature synthesis of hierarchical nickel-iron(oxy)hydroxides nanosheets on iron foam(FF-FN)with both superhydrophilicity and superaerophobicity is ***,the as-fabricated FF-FN electrode demonstrates extraordinary oxygen evolution reaction(OER)activity with an ultralow overpotential of 195 mV at 10 mA cm^(-2)and a small Tafel slope of 34 mV dec^(-1)in alkaline *** theoretical investigation indicates that the involved lattice oxygen in nickel-iron-based-oxyhydroxide during electrochemical self-reconstruction can significantly reduce the OER reaction overpotential via the dominated lattice oxygen *** rechargeable Zn-air battery assembled by directly using the as-prepared FF-FN as cathode displays remarkable cycling *** is believed that this work affords an economical approach to steer commercial Fe foam into robust electrocatalysts for sustainable energy conversion and storage systems.

关键词： electrocatalysis oxygen evolution reaction oxyhydroxide superaerophobicity superhydrophilicity

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Tuning the local coordination environment of silver(Ⅰ) coordination networks with counterions for enhanced electrocatalytic CO_(2) reduction

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science China Chemistry 2024年第5期67卷 1524-1530页

作者： Xiaofeng Cui Xueting Wang Cong Fu Bing Liu Mei-Yan Gao Tingting Kong Yujie Xiong Anhui Engineering Research Center of Carbon Neutrality The Key Laboratory of Functional Molecular SolidsMinistry of EducationAnhui Laboratory of Molecular-Based MaterialsCollege of Chemistry and Materials ScienceAnhui Normal UniversityWuhu 241002China Department of Chemical Sciences Bernal InstituteUniversity of LimerickLimerick V94 T9PXRepublic of Ireland School of Chemistry and Materials Science University of Science and Technology of ChinaHefei 230026China School of Chemical and Material Engineering Jiangnan UniversityWuxi 214122China

Very recently, the local coordination environment of active sites has been found to strongly influence their performance in electrocatalytic CO_(2) reduction by tuning the intrinsic kinetics of CO_(2) activation and intermediate stabilization. It is imperative to elucidate the mechanism for such an influence towards the rational design of efficient catalysts;however, the complex interactions between the multiple factors involved in the system make it challenging to establish a clear structure–performance relationship. In this work, we chose ion-intercalated silver(I)-based coordination networks(AgCNs) with a well-defined structure as a model platform, which enables us to understand the regulation mechanism of counterions as the counterions are the only tuning factor involved in such a system. We prepared two isostructural Ag CNs with different intercalation ions or counterions of BF_(4)^(-) and ClO_(4)^(-)(named as AgCNs-BF_(4) and AgCNs-ClO_(4)) and found that the former has a more competitive CO_(2) electroreduction performance than the latter. AgCNs-BF_(4) achieves the highest Faradaic efficiency for CO_(2) to CO of 87.1% at-1.0 V(vs. RHE) with a higher partial current density, while AgCNs-ClO_(4) exhibits only 77.2% at the same applied *** characterizations and theoretical calculation reveal that the presence of BF_(4)^(-)is more favorable for stabilizing the COOH^(*) intermediate by weakening hydrogen bonds, which accounts for the superior activity of Ag CNs-BF_(4).

关键词： electrocatalytic CO_(2) reduction coordination networks local environment counterions intercalation ions

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Far-from-equilibrium electrosynthesis ramifies high-entropy alloy for alkaline hydrogen evolution

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Journal of materials science & technology 2023年第35期166卷 234-240页

作者： Yunan Wang Hao Yang Zhe Zhang Xiangying Meng Tao Cheng Gaowu Qin Song Li Key Lab for Anisotropy and Texture of Materials(MoE) School of Material Science and EngineeringNortheastern UniversityShenyang 110819China Institute of Functional Nano&Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials&DevicesSoochow UniversitySuzhou 215123China Jiangsu Key Laboratory of Advanced Negative Carbon Technologies Soochow UniversitySuzhou 215123China Institute of Materials Intelligent Technology Liaoning Academy of MaterialsShenyang 110004China

High-entropy alloys(HEAs)provide an ideal platform for developing highly active electrocatalysts and investigating the synergy of mixed ***-from-equilibrium synthesis holds great potential for fabricating HEAs at the nanoscale by rapidly shifting the thermodynamic conditions and manipulat-ing the growth *** far-from-equilibrium synthesis of nanomaterials has been successful un-der thermochemical conditions,it is markedly challenging under electrochemical environments,as the use of an electrolyte limits the accessible temperature window and the temporal tunability of ***,we demonstrate that applying a large electrochemical overpotential would create a far-from-equilibrium condition as changing the temperature of the system by considering the equation △G=△H−T△S+nF△ψ.An electrochemical far-from-equilibrium approach is thus setup for construct-ing hierarchical and self-supporting high-entropy alloy *** large overpotential drives the simultaneous reduction of multiple cations and the subsequent formation of a single-phase *** a proof-of-concept,hierarchical Fe_(0.22)Co_(0.18)Ni_(0.18)Cr_(0.14)Cu_(0.28)was fabricated and used as an electrocatalyst for the hydrogen evolution reaction in alkaline *** noble-metal-free HEA exhibits an overpoten-tial of 84 mV at a current density of 10 mA cm^(-2),which is among the lowest even compared to noble metal-based *** work opens a new avenue for building a variety of HEAs for energy and catalysis applications.

关键词： High-entropy alloys Nanostructures Electrocatalysis Hydrogen evolution reaction Far-from-equilibrium synthesis

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Synergistic boosting the electrooxidation of biomass-based 5-hydroxymethylfurfural on cellulose-derived Co3O4/N-doped carbon catalysts

Materials Today Catalysis

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materials Today Catalysis 2024年 7卷

作者： Sun, Haixin Gao, Yingying Chen, Mengyuan Li, Ming Xia, Qinqin Liu, Yongzhuang Meng, Juan Dou, Shuo Yu, Haipeng Key Laboratory of Bio-based Material Science and Technology of Ministry of Education Northeast Forestry University Harbin150040 China School of Resources and Environmental Engineering Jiangsu University of Technology Changzhou213001 China

Catalysts play a pivotal role in the efficient conversion of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) through electrochemical oxidation. In this work, a cost-effective and highly efficient cobalt-based electrocatalyst for the synthesis of bio-based carboxylic acids was reported. By the employment of cellulose, which was dissolved in the alkaline-urea with cobalt ion, as the precursor, it derived a carbon-coated Co3O4 (Co3O4@NC) catalyst with a high specific surface area and rich porous structure. When utilized in the electrocatalytic conversion of HMF to FDCA, the catalyst exhibited exceptional yields and Faradaic efficiency which surpassed 95 %. In-situ Raman spectra unveiled that a dual-pathway process occurred on this catalyst, with part of Co3O4 serving as active sites for HMF adsorption, while other Co3O4 transformed into CoOOH during the reaction. This dual-pathway electrocatalysis facilitated the highly efficient conversion of HMF. Additionally, using bio-based alcohols/aldehydes as the feedstocks, eight carboxylic acids were successfully synthesized with yields ranging from 91.5 % to 99 %. This study presents a highly efficient electrocatalyst derived from biomass, enabling diverse bio-based carboxylic acid production with significant potential for sustainable chemical synthesis. © 2024 The Authors

关键词： Electrochemical oxidation

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Synergistic effect of Fe-Mn bimetallic sites with close proximity for enhanced CO_(2) hydrogenation performance

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Frontiers of Chemical science and Engineering 2024年第11期18卷 413-422页

作者： Haoting Liang Qiao Zhao Shengkun Liu Chongyang Wei Yidan Wang Yue Wang Shouying Huang Xinbin Ma Key Laboratory for Green Chemical Technology of Ministry of Education Collaborative Innovation Center of Chemical Science and EngineeringSchool of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China School of Materials Science and Engineering National Institute for Advanced MaterialsTKL of Metal and Molecule-Based Material ChemistryNankai UniversityTianjin 300350China Zhejiang Institute of Tianjin University Ningbo 315201China Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityFuzhou 350207China

The Fe-Mn bimetallic catalyst is a potential candidate for the conversion of CO_(2) into value-added *** interaction between the two metals plays a significant role in determining the catalytic performance,however which remains *** this study,we aim to investigate the impact of tuning the proximity of Fe-Mn bimetallic catalysts with similar nanoparticle *** its effect on the physicochemical properties of the catalysts and corresponding performance were *** was found that closer Fe-Mn proximity resulted in enhanced CO_(2) hydrogenation activity and inhibited CH4 *** physiochemical properties of prepared catalysts were characterized using X-ray diffraction,H2 temperature programmed reduction,and X-ray photoelectron spectroscopy,revealing that a closer Fe-Mn distance promoted electron transfer from Mn to Fe,thereby facilitating Fe *** adsorption behavior of CO_(2) and the identification of reaction intermediates were analyzed using CO_(2)-temperature programed desorption and in situ Fourier transform infrared spectroscopy,confirming the intimate Fe-Mn sites contributed to CO_(2) adsorption and the formation of HCOO*species,ultimately leading to increased CO_(2) conversion and hydrocarbon *** discovery of a synergistic effect at the intimate Fe-Mn sites in this study provides valuable insights into the relationship between active sites and promoters.

关键词： CO_(2)hydrogenation Fe-based catalyst proximity effect Mn promoter

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In situ formed cross-linked polymer networks as dual-functional layers for high-stable lithium metal batteries

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Journal of Energy Chemistry 2023年第4期79卷 253-262页

作者： Lei Shi Wanhui Wang Chunjuan Wang Yang Zhou Yuezhan Feng Tiekun Jia Fang Wang Zhiyu Min Ji Hu Zhigang Xue School of Materials Science and Engineering School of Environmental Engineering and ChemistryLuoyang Institute of Science and TechnologyLuoyang 471023HenanChina Key Laboratory for Material Chemistry of Energy Conversion and Storage Ministry of EducationSchool of Chemistry and Chemical EngineeringHuazhong University of Science and TechnologyWuhan 430074HubeiChina Key Laboratory of Advanced Materials Processing&Mold(Ministry of Education) National Engineering Research Center for Advanced Polymer Processing TechnologyZhengzhou UniversityZhengzhou 450002HenanChina Henan Intelligent Manufacturing Engineering Technology Research Center for Building Profile Luoyang Institute of Science and TechnologyLuoyang 471023HenanChina Henan Province International Joint Laboratory of Materials for Solar Energy Conversion and Lithium Sodium based Battery Luoyang Institute of Science and TechnologyLuoyang 471023HenanChina

Lithium-metal anodes(LMAs)have been recognized as the ultimate anodes for next-generation batteries with high energy density,but stringent assembly-environment conditions derived from the poor moisture stability dramatically hinder the transformation of LMAs from laboratory to ***,an in situ formed cross-linked polymer layer on LMAs is designed and constructed by a facile thiol-acrylate click chemistry reaction between poly(ethylene glycol)diacrylate(PEGDA)and the crosslinker containing multi thiol groups under UV *** to the hydrophobic nature of the layer,the treated LMAs demonstrate remarkable humid stability for more than 3 h in ambient air(70%relative humidity).The coating humid-resistant protective layer also possesses a dual-functional characterization as solid polymer electrolytes by introducing lithium bis(trifluoromethanesulfonyl)imide in the system in *** intimate contact between the polymer layer and LMAs reduces interfacial resistance in the assembled Li/LiFePO_(4)or Li/LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)full cell effectively,and endows the cell with an outstanding cycle performance.

关键词： Lithium-metal anode Humid-resistant protective film Solid-state polymer electrolytes Cross-linked polymers

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