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Impregnating photo-stable gold precursor onto uncalcined TS-1 to boost catalytic hydro-oxidation of propane

Science China Chemistry 2025年第4期68卷 1585-1596页

作者： Zhihua Zhang Erchuan Yang Fan Liu Kesheng Xu Yuxia Zhong Jinwei Sun Shudong Shi Xuezhi Duan Xinggui Zhou State Key Laboratory of Chemical Engineering East China University of Science and TechnologyShanghai 200237China

Immobilizing highly dispersed Au nanoparticles onto titanium silicalite-1(TS-1)by a simple impregnation method under light is still a challenging *** this work;a high photostable Au precursor protected by thiol ligands was firstly synthesized;and the as-prepared Au precursor displayed excellent stability under light for over 30 days;while the Au precursor without thiol ligands formed precipitates after just 2 h under ***;the Au precursor protected by thiol ligands was immobilized on the external surface of uncalcined TS-1(i.e.;TS-1-B)by the incipient wetness impregnation method(IWI method)to prepare Au/TS-1-B *** activity of as-prepared Au/TS-1-B catalyst in the hydro-oxidation of propane to acetone was 1.4 times higher than that of the catalyst prepared by the deposition-precipitation urea method(DPU method).The structures of the Au/TS-1-B catalysts prepared by different methods were analyzed by multiple *** to the Au/TS-1-B catalyst prepared by the DPU method;the Au/TS-1-B catalyst synthesized by the IWI method exhibited a narrower size distribution of Au nanoparticles and had more small Au particles(<2 nm);which is the main reason for its superior ***;the effects of gold loadings;reaction temperature and Si/Ti molar ratio on the catalytic performance of the Au/TS-1-B catalyst prepared by the IWI method were also *** addition;the Au/TS-1-B catalyst prepared by the IWI method also exhibited excellent stability for over 140 h.

关键词： hydro-oxidation of propane acetone Au-Ti bifunctional catalysts IWI method thiol ligands stability

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Intrinsic pentagon defect engineering in multiple spatial-scale carbon frameworks for efficient triiodide reduction

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Journal of Energy Chemistry 2024年第8期95卷 20-28,I0002页

作者： Siyi Hou Xuedan Song Chang Yu Jiangwei Chang Yiwang Ding Yingbin Liu Xiubo Zhang Weizhe Liu Jieshan Qiu State Key Lab of Fine Chemicals Liaoning Key Lab for Energy Materials and Chemical EngineeringFrontier Science Center for Smart MaterialsSchool of Chemical EngineeringDalian University of TechnologyDalian 116024LiaoningChina Liaoning Key Lab for Energy Materials and Chemical Engineering Frontier Science Center for Smart MaterialsSchool of ChemistryDalian University of TechnologyDalian 116024LiaoningChina State Key Laboratory of Chemical Resource Engineering College of Chemical EngineeringBeijing University of Chemical TechnologyBeijing 100029China

Intrinsic topological defect engineering has been proven as a promising strategy to elevate the electrocatalytic activity of carbon ***,the controllable construction of high-density and specific topological defects in carbon frameworks to reveal the relationship between reactivity and defect structure remains a challenging ***,the intrinsic pentagon carbon sites that can favor electron overflow and enhance their binding affinity towards the intermediates of catalytic reaction are firstly presented by the work function and the p-band center *** experimentally verify this,the cage-opening reaction of fullerene is proposed and utilized for synthesizing carbon quantum dots with specific pentagon configuration(CQDs-P),subsequently utilizing CQDs-P to modulate the micro-scale defect density of three-dimensional reduced graphene oxide(rGO)viaπ-π*** multiple spatial-scale rGO-conjugated CQDs-P structure simultaneously possesses abundant pentagon and edge defects as catalytic active sites and long-range-orderedπelectron delocalization system as conductive *** defects-rich CQDs-P/rGO-4 all-carbon-based catalyst exhibits superb catalytic activity for triiodide reduction reaction with a high photoelectric conversion efficiency of 8.40%,superior to the Pt reference(7.97%).Theoretical calculations suggest that pentagon defects in the carbon frameworks can promote charge transfer and modulate the adsorption/dissociation behavior of the reaction intermediates,thus enhancing the electrocatalytic activity of the *** work confirms the role of intrinsic pentagon defects in catalytic reactions and provides a new insight into the synthesis of defects-rich carbon catalysts.

关键词： Defect engineering Pentagon carbon Carbon quantum dots Electrocatalytic activity Triiodide reduction

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An effective'salt in dimethyl sulfoxide/water'electrolyte enables high-voltage supercapacitor operated at-50℃

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Journal of Energy Chemistry 2024年第6期93卷 361-367,I0009页

作者： Yingbin Liu Chang Yu Xuedan Song Siyi Hou Shuqin Lan Jinhe Yu Yuanyang Xie Jieshan Qiu State Key Lab of Fine Chemicals Frontier Science Center for Smart MaterialsSchool of Chemical EngineeringLiaoning Key Lab for Energy Materials and Chemical EngineeringDalian University of TechnologyDalian 116024LiaoningChina School of Chemistry Frontier Science Center for Smart MaterialsLiaoning Key Lab for Energy Materials and Chemical EngineeringDalian University of TechnologyDalian 116024LiaoningChina College of Chemical Engineering State Key Laboratory of Chemical Resource EngineeringBeijing University of Chemical TechnologyBeijing 100029China

Compared with organic electrolytes,aqueous electrolytes exhibit significantly higher ionic conductivity and possess inherent safety features,showcasing unique advantages in ***,challenges remain for low-salt aqueous electrolytes operating at high voltage and low ***,we report a low-salt(0.87 m,m means mol kg^(-1))'salt in dimethyl sulfoxide/water'hybrid electrolyte with non-flammability via hybridizing aqueous electrolyte with an organic co-solvent of dimethyl sulfoxide(hydrogen bond acceptor).As a result,the 0.87 m hybrid electrolyte exhibits enhanced electrochemical stability,a freezing temperature below-50℃,and an outstanding ionic conductivity of 0.52mS cm~(-1)at-50℃.Dimethyl sulfoxide can anchor water molecules through intermolecular hydrogen bond interaction,effectively reinforcing the stability of water in the hybrid ***,the interaction between dimethyl sulfoxide and water molecules diminishes the involvement of water in the generation of ordered ice crystals,finally facilitating the low-temperature performance of the hybrid *** paired with the 0.87 m'salt in dimethyl sulfoxide/water'hybrid electrolyte,the symmetric supercapacitor presents a 2.0 V high operating voltage at 25℃,and can operate stably at-50℃.Importantly,the suppressed electrochemical reaction of water at-50℃further leads to the symmetric supercapacitor operated at a higher voltage of 2.6 *** modification strategy opens an effective avenue to develop low-salt electrolytes for high-voltage and low-temperature aqueous supercapacitors.

关键词： Dimethyl sulfoxide Co-solvent High voltage Low temperature Supercapacitors

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Synergistic effect of Co and Co_(6)Mo_(6)C for electroreduction of nitrate to ammonia on Co-MOF derived Co_(6)Mo_(6)C/Co/NC

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Nano Research 2024年第7期17卷 5807-5816页

作者： Xinyan Wang Yue Cao Yan Hai Xiaoman Li Min Luo State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering School of Chemistry and Chemical EngineeringNingxia UniversityYinchuan 750021China

Electrocatalytic nitrate reduction reaction(e-NO_(3)RR)offers a promising alternative method for nitrogen cycling and ammonia(NH3)production under ambient ***,the method is still in the dilemma of lowering the reaction overpotential and increasing the reaction *** successfully developed the composition-adjustable Co_(6)Mo_(6)C/Co/N-doped carbon(NC)catalysts by in situ carbonization of Co-based metal-organic framework(MOF)with the constrained phosphomolybdic *** adjusting the ratio of Co0 and Co_(6)Mo_(6)C,Co_(6)Mo_(6)C/Co/NC-3 could satisfy both NO_(3)−conversion at low potential and NH_(x)hydrogenation,and synthesize ammonia efficiently through the synergistic effect of Co0 and Co_(6)Mo_(6)*** achieved an ammonia yield rate as 1233.2μg·h^(−1)·mgcat^(−1)and Faradaic efficiency of NH4+93.6%at−0.33 V *** hydrogen electrode(RHE).Importantly,density functional theory(DFT)calculations and experimental results have demonstrated for the first time the excellent adsorption of nitrite(NO_(2)^(−))by the Mo sites of Co_(6)Mo_(6)C during e-NO_(3)RR,avoiding the undesirable accumulation of NO_(2)^(−).

关键词： synergistic effect nitrate electroreduction Co_(6)Mo_(6)C ammonia synthesis

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Amine-functionalized metal-organic frameworks loaded with Ag nanoparticles for cycloaddition of CO_(2)to epoxides

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Frontiers of chemical Science and engineering 2024年第11期18卷 193-203页

作者： Huiyu Fu Jiewen Wu Changhai Liang Xiao Chen State Key Laboratory of Fine Chemicals&Laboratory of Advanced Materials and Catalytic Engineering School of Chemical EngineeringDalian University of TechnologyDalian 116024China

With the advantages of low raw material cost and 100%atom utilization,the synthesis of high value-added chemical product cyclic carbonates by the cycloaddition of CO_(2)to epoxides has become one of the most prospective approaches to achieve the industrial utilization of CO_(2).In the reported catalytic systems,the complexity of the catalyst synthesis process,high cost,separation difficulties,and low CO_(2)capture limit the catalytic efficiency and its large-scale *** this paper,Ag nanoparticles loaded on polyethyleneimine(PEI)-modified UiO-66-NH_(2)(Ag/PEI@UiO-66-NH_(2))are successfully synthesized by in situ immersion *** Ag nanoparticles and the amino groups on the surfaces of PEI@UiO-66-NH_(2)contribute to the adsorption of CO_(2)and polarization of C–O bonds in epoxides,thereby boosting the conversion capability for the CO_(2)cycloaddition *** the amount of propylene oxide of 0.25 mol and the catalyst dosage of 1%of the substrate,the yield and selectivity of propylene carbonate are up to 99%.In addition,the stability and recyclability of Ag/PEI@UiO-66-NH_(2)catalyst are *** Ag/PEI@UiO-66-NH_(2)catalyst also demonstrates a wide range of activity and distinctive selectivity toward cyclo-carbonates in the cycloaddition of CO_(2)to *** work provides a guide to designing a highly efficient catalyst for in situ capture and high-value utilization of CO_(2)in industrial applications.

关键词： cycloaddition CO_(2)capture cyclic carbonates amine-functionalized UiO-66-NH_(2) Ag NPs

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Tailoring NH_(4)^(+)storage by regulating oxygen defect in ammonium vanadate

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Green Energy & Environment 2024年第7期9卷 1171-1182页

作者： Yanyan Liu Ziyi Feng Hanmei Jiang Xueying Dong Changgong Meng Yifu Zhang State Key Laboratory of Fine Chemicals School of Chemical EngineeringDalian University of TechnologyDalian116024China College of Environmental and Chemical Engineering Dalian UniversityDalian116622China

Defect engineering is an effective strategy for modifying the energy storage materials to improve their electrochemical ***,the impact of oxygen defect and its content on the electrochemical performances in the burgeoning aqueous NH_(4)^(+)storage field remains ***,for the first time in this work,an oxygen-defective ammonium vanadate[(NH_(4))_(2)V_(10)O_(25)·8H_(2)O,denoted as Od-NHVO]with a novel 3D porous flower-like architecture was achieved via the reduction of thiourea in a mild reaction condition,which is a facile method that can realize the intention to regulate the oxygen defect content,with the capability of *** as-prepared Od_M-NHVO with moderate oxygen defect content can deliver a stable specific capacitance output(505 F g^(-1),252 mAh g^(-1)at 0.5 A g^(-1)with~80% capacitance retention after 10,000 cycles),which benefits from extra active sites,unimpeded NH_(4)^(+)-migration path and relatively high structure *** contrast,low oxygen defect content will lead to the torpid electrochemical reaction kinetics while too high content of it will reduce the chargestorage capability and induce structural *** superior NH_(4)^(+)-storage behavior is achieved with the reversible intercalation/deintercalation process of NH_(4)^(+)accompanied by forming/breaking of hydrogen *** expected,the assembled flexible OdM-NHVO//PTCDI quasi-solid-state hybrid supercapacitor(FQSS HSC)also exhibits high areal capacitance,energy density and reliable *** work provides a new avenue for developing materials with oxygen-deficient structure for application in various aqueous non-metal cation storage systems.

关键词： Ammonium vanadate Oxygen defect Ammonium-ion storage Hybrid supercapacitors Electrochemical performance

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Study on the adsorption performance and regeneration of lignin-derived graphitic carbon for H_(2)S

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Particuology 2024年第11期94卷 197-210页

作者： Fen Li Ruiying Wang Ying Yang Menglong Zheng Qiushuang Li Dongdong Yang Huiyu Chen Key Laboratory of Green Chemical Engineering and Technology of College of Heilongjiang Province School of Materials Science and Chemical EngineeringHarbin University of Science and TechnologyHarbin150080China

In pursuit of effective adsorption materials for malodorous gases such as H_(2)S and to broaden the utilization avenues of lignin waste,this study employed the direct pyrolysis method to synthesize three types of alkali lignin graphitized carbons,namely C-800,KC-700,and *** them,KEC-700 exhibits a high specific surface area of 1672.9 m^(2)/g,significantly superior H_(2)S adsorption performance compared to other materials,an adsorption breakthrough time of up to 220 min,and a sulfur capacity of 67.1 mg/*** analysis showed that the more oxygen-containing functional groups of lignin charcoal and the larger specific surface area facilitated the adsorption of H_(2)*** reaching adsorption saturation,the degree of graphitization of lignin carbon *** H_(2)S adsorption products primarily manifest as elemental sulfur and sulfate within the pores of lignin carbon measuring less than 2 *** thermal regeneration,the charcoal effectively eliminates the elemental sulfur adsorption ***,sulfate removal proved unsatisfactory,as the adsorption efficiency of KEC-700 following two thermal regenerations was approximately 41%of that observed for fresh samples.

关键词： Hydrogen sulfide Alkali lignin Lignin carbon Regeneration

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Polymer engineering for electrodes of aqueous zinc ion batteries

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Journal of Energy Chemistry 2024年第4期91卷 345-369页

作者： Zhi Peng Zemin Feng Xuelian Zhou Siwen Li Xuejing Yin Zekun Zhang Ningning Zhao Zhangxing He Lei Dai Ling Wang Chao Lu School of Chemical Engineering North China University of Science and TechnologyTangshan 063210HebeiChina State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical TechnologyBeijing 100029China

With the increasing demand for scalable and cost-effective electrochemical energy storage,aqueous zinc ion batteries(AZIBs)have a broad application prospect as an inexpensive,efficient,and naturally secure energy storage ***,the limitations suffered by AZIBs,including volume expansion and active materials dissolution of the cathode,electrochemical corrosion,irreversible side reactions,zinc dendrites of the anode,have seriously decelerated the civilianization process of ***,polymers have tremendous superiority for application in AZIBs attributed to their exceptional chemical stability,tunable structure,high energy density and outstanding mechanical *** the expanding applications of AZIBs and the superiority of polymers,this comprehensive paper meticulously reviews the benefits of utilizing polymeric applied to cathodes and anodes,*** begin with,with adjustable structure as an entry point,the correlation between polymer structure and the function of energy storage as well as optimization is deeply investigated in respect to the ***,depending on the diversity of properties and structures,the development of polymers in AZIBs is summarized,including conductive polymers,redox polymers as well as carbon composite polymers for cathode and polyvinylidene fluoride-,carbonyl-,amino-,nitrile-based polymers for anode,and a comprehensive evaluation of the shortcomings of these strategies is ***,an outlook highlights some of the challenges posed by the application of polymers and offers insights into the potential future direction of polymers in *** is designed to provide a thorough reference for researchers and developers working on polymer for AZIBs.

关键词： Aqueous zinc ion batteries Polymer Multi-function Anode protection Energy storage

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Cascade refrigeration system synthesis based on hybrid simulated annealing and particle swarm optimization algorithm

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Chinese Journal of chemical engineering 2023年第6期58卷 244-255页

作者： Danlei Chen Yiqing Luo Xigang Yuan Chemical Engineering Research Center School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300350China State Key Laboratory of Chemical Engineering Tianjin UniversityTianjin 300350China

Cascade refrigeration system(CRS)can meet a wider range of refrigeration temperature requirements and is more energy efficient than single-refrigerant refrigeration system,making it more widely used in low-temperature industry *** synthesis of a CRS with simultaneous consideration of heat integration between refrigerant and process streams is challenging but promising for significant cost saving and reduction of carbon *** study presented a stochastic optimization method for the synthesis of *** MINLP model was formulated based on the superstructure developed for the CRS,and an optimization framework was proposed,where simulated annealing algorithm was used to evolve the numbers of pressure/temperature levels for all sub-refrigeration systems,and particle swarm optimization algorithm was employed to optimize the continuous *** effectiveness of the proposed methodology was verified by a case study of CRS optimization in an ethylene plant with 21.89%the total annual cost saving.

关键词： Optimal design Process systems Particle swarm optimization Simulated annealing Mathematical modeling

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Regulating the oxidation state of Pd to enhance the selective hydrogenation for 5-hydroxymethylfurfural

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Chinese Journal of chemical engineering 2024年第8期72卷 60-68页

作者： Xin Li Yue Ma Xuning Wang Jianguo Wu Dong Cao Daojian Cheng State Key Laboratory of Organic-Inorganic Composites and College of Chemical Engineering Beijing University of Chemical TechnologyBeijing 100029China

The highly selective hydrogenation of 5-hydroxymethylfurfural to 2,5-dihydroxymethylfuran is an important reaction in the field of biomass hydrogenation,because it is a bridge between biomass resources and chemical ***,we precisely constructed carbon nitride supported Pd-based catalysts by a simple impregnation-reduction *** changing the reduction temperature,catalysts with different oxidation state could be precisely ***,the important correlation between the ratio of Pd^(0)/Pd^(2+)and catalytic activity is revealed during the selective hydrogenation of *** Pd/g—C_(3)N_(4)—300 catalyst with a Pd^(0)/Pd^(2+)ratio of 3/2 showed the highest catalytic activity,which could get 96.9%5-hydroxymethylfurfural conversion and 90.3%2,5-dihydroxymethylfuran *** density functional theory calculation revealed that the synergistic effect between Pd0and Pd2+in Pd/g—C_(3)N_(4)—300 system could boost the adsorption of the substrate and the dissociation of *** this work,we highlight the important correlation between metal oxidation state and catalytic activity,which provides valuable insights for the rational design of precious metal catalysts for hydrogenation reactions.

关键词： Pd/g-C_(3)N_(4) Selective hydrogenation 5-hydroxymethylfurfural 2,5-dihydroxymethylfuran Oxidation state

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