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

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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AuPt bimetallic nanoalloys supported on SBA-15:A superior catalyst for quinoline selective hydrogenation in water

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Nano Research 2022年第3期15卷 1796-1802页

作者： Jianbo Zhao Haifeng Yuan Guang Yang Yingfan Liu Xiaomei Qin Zheng Chen Cheong Weng-Chon Liming Zhou Shaoming Fang School of Material and Chemical Engineering Zhengzhou University of Light IndustryZhengzhou 450001China Key Laboratory of Functional Molecular Solids Ministry of EducationAnhui Key Laboratory of Molecule-Based MaterialsCollege of Chemistry and Materials ScienceAnhui Normal UniversityWuhu 241000China Department of Physics and Chemistry Faculty of Science and TechnologyUniversity of MacaoMacao SARChina

The structure and size of bimetallic catalysts play a crucial role in many important chemical *** synthesis of bimetallic nanoparticles avoiding overgrowth and aggregation can be achieved by surfactants,which are always detrimental to catalytic performances and understanding of structure-property *** of surface-clean bimetallic catalysts with uniform size and well-defined structure is still *** the Au-Pt bimetallic nanoparticles immobilized on SBA-15 were prepared by facile adsorption-reduction *** showed that Au-Pt bimetallic nanoparticles were evenly confined within the mesopores of SBA-15,possessing the uniform size of 6.0 nm and existing in the form of alloy *** the first time the Au-Pt bimetallic nanoalloys with Au-to-Pt molar ratio of 5:1(Au5Pt1@SBA-15)exhibited a lot higher activity than monometallic Au@SBA-15 and Pt@SBA-15 catalysts with excellent selectivity towards 1,2,3,4-tetrahydroquinoline for chemoselective hydrogenation of quinoline in water under very mild *** was superior to other heterogeneous catalysts reported to *** observed properties were related to the synergic effect between Au and *** Pt sites of high electron density originated from the electron transfer between Au and Pt enhanced the ability of H_(2) dissociation and then provided a new and main approach to H_(2) splitting,while the Au sites accounted for the adsorption and activation of *** precise synthetic strategy will be very helpful to explore surface-clean gold-based bimetallic catalysts with high performance for selective hydrogenations.

关键词： gold platinum bimetallic catalyst quinoline selective hydrogenation

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Soft-Template Hydrothermal Synthesis of N, B Co-Doped Walnut-Shaped Porous Carbon Sphere with Hydrophilic Surface for Supercapacitor

SSRN

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SSRN 2023年

作者： Xu, Zhou Wu, Zhenwei Chi, Junlin Lei, E. Liu, Yuxuan Yin, Yu Yang, Zheng Ma, Chunhui Li, Wei Luo, Sha Liu, Shouxin Key Laboratory of Bio-based Material Science & Technology Northeast Forestry University Ministry of Education Heilongjiang Harbin150040 China

N, B co-doped walnut-shaped porous carbon spheres (NBCs) were prepared by soft-template hydrothermal carbonization of glucosamine, boric acid and block copolymer (P123). The NBCs formed a three-dimensional interconnected structure, and were doped with nitrogen in the forms of pyridine N (N-6), pyrrole N (N-5), graphite N (N-Q), nitrogen oxide (N-O) or N-B and boron in the forms of CB3, CB2O, CBO2 or B-N. Chemical vapor oxidation with controllable low concentration nitric acid was used to transform its super-hydrophobicity into well-hydrophilicity. The porous carbon sphere with hydrophilic surface maintained a relatively complete walnut-shaped structure, high specific surface area and stable heteroatom doping, and exhibited an improved specific capacitance of 281 F·g-1 at a current density of 0.2 A·g-1 and rate performance of 75 % at 5 A·g-1. The assembled symmetrical supercapacitor showed a high energy density of 6.56 W·h·kg-1 at 0.1 A·g-1 and superb cycling stability of 95% after 5000 cycles at 2 A·g-1. For electrode materials, walnut-shaped structure with short electron and ion transport paths enhanced the utilization efficiency. Heteroatom doping improved the conductivity and reactivity. High specific surface area contributed to the storage and transport of ions. Hydrophilic surface facilitated the penetration and mass transfer of ion and electrolyte. © 2023, The Authors. All rights reserved.

关键词： Supercapacitor

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引用

Chinese Chemical Letters 2023年第1期34卷 203-205页

作者： Mingjun Zhong Qimeng Wu Liang Ma Jie Li Yifan Wang Yansong Wang Xin Li Yajie Zhang Jingtao Lü Yongfeng Wang Center for Carbon-based Electronics and Key Laboratory for the Physics and Chemistry of Nanodevices Department of ElectronicsPeking UniversityBeijing 100871China Key Laboratory for Microstructural Material Physics of Hebei Province School of ScienceYanshan UniversityQinhuangdao 066004China School of Physics Institute for Quantum Science and Engineeringand Wuhan National High Magnetic Field CenterHuazhong University of Science and TechnologyWuhan 430074China Beijing Academy of Quantum Information Sciences Beijing 100193China Institute of Spin Science and Technology South China University of TechnologyGuangzhou 511442China

Spin properties of organic molecules have attracted great interest for their potential applications in spintronic devices and quantum ***-tetraphenyl porphyrin(Fe TPP)is of particular interest for its robust magnetic properties on metallic *** TPP is prepared in vacuum via on-surface *** structure and spin-related transport properties are characterized by low-temperature scanning tunneling microscope and spectroscopy at 0.5 *** functional theory calculations are performed to understand molecular adsorption and spin distribution on Au(111).The molecular structure of Fe TPP is distorted upon adsorption on the *** excitations of Fe TPP are observed on the Fe atom and high pyrrole groups in differential conductance *** calculated spin density distribution indicates that the electron spin of Fe TPP is mainly distributed on the Fe *** atomic transmission calculation indicates that electrons transport to substrate is mediated through Fe atom,when the tip is above the high pyrrole group.

关键词： Spintronics Spin excitation Atomic transmission Fe-tetraphenyl porphyrin STM

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