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Combined effects of sea urchin-like structure and mixed Cu^(+)/Cu^(0)states on promoting C_(2)formation in electrocatalytic CO_(2)reduction

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Frontiers of chemical science and Engineering 2024年第3期18卷 63-73页

作者： Mengqing Shan Dongsheng Lu Jiatong Dong Shen Yan Jinyu Han Hua Wang Collaborative innovation center of chemical science and Engineering Key Laboratory for Green Chemical Technology of the Ministry of EducationSchool of Chemical Engineering and TechnologyTianjin UniversityTianjin300354China

Surface engineering and Cu valence regulation are essential factors in improving the C_(2)selectivity during the electrochemical reduction of CO_(2).Herein,we present a sea urchin-like CuO/Cu_(2)O catalyst derived from rhombic dodecahedra Cu_(2)O through one-step oxidation/etching method where the mixed Cu^(+)/Cu^(0)states are formed via in situ reduction during *** combined effects of the morphology and the mixed Cu^(+)/Cu^(0)states on C–C coupling are evaluated by the Faradaic efficiency of C_(2)and the C_(2)/C1 ratio obtained in an H-cell.R-Cu^(O)/Cu_(2)O exhibited 49.5%Faradaic efficiency of C_(2)with a C_(2)/C1 ratio of 3.1 at−1.4 V *** hydrogen electrode,which are 1.5 and 3.2 times higher than those of R-Cu_(2)O,*** a flow-cell,68.0%Faradaic efficiency of C_(2)is achieved at a current density of 500 mA·cm^(−2).The formation of the mixed Cu^(+)/Cu^(0)states was confirmed by in situ Raman ***,the sea urchin-like structure provides more active sites and enables faster electron *** a result,the excellent C_(2)production on R-CuO/Cu_(2)O is primarily attributed to the synergistic effects of the sea urchin-like structure and the stable mixed Cu^(+)/Cu^(0)***,this work presents an integrated strategy for developing Cu-based electrocatalysts for C_(2)production through electrochemical CO_(2)reduction.

关键词： CO_(2)electrolysis sea urchin-like structure Cu^(+)/Cu^(0) C_(2)products

CO_(2) hydrogenation to methanol over the copper promoted In_(2)O_(3) catalyst

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Journal of Energy Chemistry 2024年第6期93卷 135-145,I0004页

作者： Rui Zou Chenyang Shen Kaihang Sun Xinbin Ma Zhuoshi Li Maoshuai Li Chang-Jun Liu School of chemical Engineering and Technology Tianjin UniversityTianjin 300350China Collaborative innovation center of chemical science&Engineering Tianjin UniversityTianjin 300072China

The metal promoted In_(2)O_(3) catalysts for CO_(2) hydrogenation to methanol have attracted wide attention because of their high activity with high methanol ***,there was still no experimental confirmation if copper could be a good promoter for In_(2)O_(3).Herein,the Cu promoted In_(2)O_(3) catalyst was prepared using a deposition-precipitation *** prepared Cu/In_(2)O_(3) catalyst shows significantly higher CO_(2) conversion and space time yield(STY)of methanol,compared to the un-promoted In_(2)O_(3) *** loading of Cu facilitates the activation of both H_(2) and CO_(2) with the interface between the Cu cluster and defective In_(2)O_(3) as the active *** Cu/In_(2)O_(3) catalyst takes the CO hydrogenation pathway for methanol synthesis from CO_(2) *** exhibits a unique size effect on the CO *** temperatures below 250℃,CO adsorption on Cu/In_(2)O_(3) is stronger than that on In_(2)O_(3),causing higher methanol *** increasing temperatu res,the Cu catalyst aggregates,which leads to the formation of weak CO adsorption site and causes a decrease in the methanol *** with other metal promoted In_(2)O_(3) catalysts,it can be concluded that the catalyst with stronger CO adsorption possesses higher methanol selectivity.

关键词： CO_(2)hydrogenation Methanol Cu In_(2)O_(3) CO Selectivity DFT

Graphene from microwave-initiated upcycling of waste polyethylene for electrocatalytic reduction of chloramphenicol

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Chinese chemical Letters 2024年第4期35卷 187-192页

作者： Qiang Cao Xue-Feng Cheng Jia Wang Chang Zhou Liu-Jun Yang Guan Wang Dong-Yun Chen Jing-Hui He Jian-Mei Lu College of Chemistry Chemical Engineering and Materials ScienceCollaborative Innovation Center of Suzhou Nano Science and TechnologySoochow UniversitySuzhou 215123China

Waste polyolefin plastics, accounting for 50% of all plastic waste, represent a tremendously unexploited carbon source. Efficiently upcycling polyolefin waste into value-added carbon materials for waste water treatment avoiding using noble metals is challenging but economically and environmentally sustainable. In this work, MAX-Ti_(3)AlC_(2) supported Fe selectively catalyzes polyolefin into few-layered graphene in 5 min under microwave treatment. Graphene and MAX supported Fe(Fe@MLC) can completely(99.9%)degrade chloramphenicol(CAP) within 60 min, retain robust after 10 cycles and work efficiently at a wide p H range(3.87–13.03), avoiding the usage of noble metal. Moreover, the electrochemical active surface area(ECSA) of Fe@MLC is 2.7 times higher than that of commercial Pt/C. This work provides a cheap and efficient catalyst that promotes deconstruction of plastic wastes and indirectly degrades antibiotics thereby realizes the treatment of waste water with waste plastic.

关键词： Microwave Ti_(3)AlC_(2) Electrochemistry Dechlorination Chloramphenicol

Molecular surface functionalization of In_(2)O_(3) to tune interfacial microenvironment for enhanced catalytic performance of CO_(2) electroreduction

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Nano Research 2024年第3期17卷 1242-1250页

作者： Suwen WangQiang GaoCui Xu Shuai Jiang Mengyang Zhang Xianjun Yin Hui-Qing Peng Bin Liu Yu-Fei Song State Key Laboratory of chemical Resource Engineering Beijing Advanced Innovation Center for Soft Matter Science and EngineeringCollege of ChemistryBeijing University of Chemical TechnologyBeijing 100029China

Indium-based materials(e.g.,In_(2)O_(3))are a class of promising non-noble metal-based catalysts for electroreduction of carbon dioxide(CO_(2)).However,competitive hydrogen reduction reaction(HER)on indium-based catalysts hampers CO_(2) reduction reaction(CO_(2)RR)*** herein tune the interfacial microenvironment of In_(2)O_(3) through chemical graft of alkyl phosphoric acid molecules using a facile solution-processed strategy for the first time,which is distinguished from other researches that tailor intrinsic activity of In_(2)O_(3) *** surface functionalization of alkyl phosphoric acids over In_(2)O_(3) is demonstrated to remarkably boost CO_(2) *** example,octadecylphosphonic acid modified In_(2)O_(3) exhibits Faraday efficiency for H_(2) H_(2) H_(2)(FE)of as low as 6.6%and FEHCOOH of 86.5%at-0.67 V ***,which are far superior to parent In_(2)O_(3) counterparts(FE of 24.0%and FEHCOOH of 63.1%).Moreover,the enhancing effect of alkyl phosphoric acid functionalization is found to be closely related to the length of alkyl *** virtue of comprehensive experimental characterizations and molecular dynamics simulations,it is revealed that the modification of alkyl phosphoric acids significantly alters the interface microenvironment of the electrocatalyst,which changes the electrocatalyst surface from hydrophilic and aerophobic to hydrophobic and *** this case,the water molecules are pushed away and more CO_(2) molecules are trapped,increasing local CO_(2) concentration at In_(2)O_(3) active sites,thus leading to the significantly enhanced CO_(2)RR and suppressed *** work highlights the importance of regulating the interfacial microenvironment of inorganic catalysts by molecular surface functionalization as a means for promoting the electrochemical performance in electrosynthesis and beyond.

关键词： carbon dioxide(CO_(2))electroreduction interfacial microenvironment molecular surface functionalization In_(2)O_(3)catalyst water and CO_(2)diffusion

Regulation of solvation structure and the cooperation environment of potassium bonds for wider-temperature adaptive potassium storage

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Rare Metals 2024年第4期43卷 1610-1621页

作者： Bing-Bing Liu Yi-Hui Liu You-Bin Zhang Zhen-Guo Qi Guo-Hui Qin State Key Laboratory Base for Eco-chemical Engineering College of Chemical EngineeringQingdao University of Science and TechnologyQingdao266042China Shandong Synergetic innovation center of Ecological and chemical Engineering Qingdao266042China

Antimony selenide(Sb_(2)Se_(3))is one of the perspective candidates for potassium-ion batteries due to its advanced virtues stem including featured high capacity,fertile reserves and the relative narrow band *** the unique advantages,it is still plagued by the unstable interface compatibility and poor wider-temperature *** optimization of microstructure and the construction of inorganic-organic hybrids with a low desolvation barrier and rapid kinetics behaviors are efficient to address these *** Sb_(2)Se_(3)nanorods enclosed by the S-doped carbon layer(SC),further crosslinked by the poly(N-isopropylacrylamide)(PM)film(PM@Sb_(2)Se_(3)@SC),were artificially fabricated,and it displays the enrichment ion aggregated model as well as contacted ion pair state,the well-tailored cooperation environment of potassium bonds,assuring a homogeneous potassium deposition and an excellent widertemperature *** complicated experimental studies and theoretical calculations authenticate the synergistic effects of geometric conformation and compositional design for the tremendously enhanced potassium ***,the full device over PM@Sb_(2)Se_(3)@SC anode and the potassium Prussian blue cathode manifests impressively durable cycling life and wider-temperature adaptability,verifying the glorious contribution from the finely manipulation in solvation structure and potassium bonds to enhancing the potassium storage behaviors.

关键词： Anode Sb_(2)Se_(3) rods Interface compatibility Inorganic-organic electrode Potassium ion battery

Research progress on simulation of multiscale mass transfer processes in gas-solid system by computational mass transfer

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Particuology 2024年第7期90卷 478-492页

作者： Xu Li Yaohui Wang Leifu Li Runye Zhang Hailun Ren Wenbin Li Zhongli Tang Donghui Zhang The Research center of chemical Engineering School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China The Department of chemical Engineering Tianjin Renai CollegeTianjin 301636China Collaborative innovation center of chemical science and Engineering(Tianjin) School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China

Particle-fluid system is one of the most popular systems in chemical *** to complex interface structure and high-velocity turbulence,the momentum and mass transfer exhibit nonlinear characteristics,which pose a great challenge for further study and *** solve this problem,computational mass transfer(CMT)emerged and has been proved to be effective in deeply exploring the mass transfer behavior of particle-fluid ***,this paper reviews recent gas-solid numerical studies of turbulence issues from empirical to theoretical,then discusses interphase mass transfer rate models and the interfacial interaction ***,the present study particularly reviews researches on mass transfer process of fixed and fluidized regime by CMT,providing reliable analysis of turbulent anisotropy diffusivity as well as multiscale structure and presenting theoretical instruction for the industrial optimization of mass transfer processes in chemical engineering.

关键词： Fixed bed Fluidized bed Computational mass transfer Turbulent mass diffusion Multiscale Anisotropy

Donor-acceptor covalent organic frameworks-confined ultrafine bimetallic Pt-based nanoclusters for enhanced photocatalytic H_(2)generation

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Nano Research 2024年第7期17卷 5835-5844页

作者： Yu Liu Yawen Shi Hua Wang Shengbo Zhang Collaborative innovation center of chemical science and Engineering(Tianjin) Key Laboratory for Green Chemical Technology of the Ministry of EducationSchool of Chemical Engineering and TechnologyTianjin UniversityTianjin 300350China School of Environmental science and Engineering Tianjin Key Laboratory of Biomass/Wastes UtilizationTianjin UniversityTianjin 300350China

Photocatalytic hydrogen generation from hydrogen storage media is an effective and promising approach for the green hydrogen industry as well as for achieving carbon neutrality ***,the lower photocatalytic efficiency due to the limited light trapping capacity,low electron transfer rate,and severe aggregation of nanoparticles caused by high surface energy seriously restricts their practical ***,we constructed a series of donor–acceptor(D–A)type covalent organic frameworks to confine ultrafine bimetallic Pt-based nanoclusters for photocatalytic hydrogen generation from ammonia borane(AB)*** visible light irradiation at 20℃,PtCo_(2)@covalent organic framework(COF)showed the highest photocatalytic activity with a turnover frequency(TOF)of 486 min−*** and density functional theory(DFT)calculations reveal that the high catalytic activity is mainly attributed to the strong electronic interactions between D–A type COF and ultrafine PtCo_(2)***,the D–A type COF can significantly enhance the light-trapping ability by fine-tuning the electron-acceptor type in the framework,and accelerate the photogenerated electron transfer from D–A type COF to PtCo_(2)nanocluster,which promotes the adsorption and activation of H_(2)O and AB molecules and accelerates hydrogen ***,PtCo_(2)@COF also exhibited ultra-high durability due to the significantly enhanced resistance to nanocluster aggregation caused by the nanopore confinement effect of D–A type *** believe that this work will provide a theoretical guide for the rational design of efficient D–A COFbased catalysts for photocatalysis.

关键词： light trapping electron transfer donor-acceptor covalent organic frameworks(D-A COFs) bimetallic nanoclusters photocatalysis

Central aromatic-core fluorination in non-fullerene acceptor advances binary organic solar cells to a record efficiency of 19.7%

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science China Materials 2024年第8期67卷 2713-2714页

作者： Ming Zhang Zhi-Guo Zhang State Key Laboratory of Organic/Inorganic Composites Beijing Advanced Innovation Center for Soft Matter Science and EngineeringBeijing University of Chemical TechnologyBeijing 100029China

Organic solar cells(OSCs)hold great promise for the conversion of solar energy into electricity,showing advantages such as lightweight,flexibility,semi-transparency,and solution *** field has witnessed significant adv... 详细信息

关键词： aromatic acceptor transparency

Flexible Organic Crystal with Two-Dimensional Elastic Bending and Recoverable Plastic Twisting for Circularly Polarized Luminescence

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CCS Chemistry 2024年第6期6卷 1439-1447页

作者： Wenjie Kuang Bo Jing Songgu Wu Junbo Gong State Key Laboratory of chemical Engineering School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072 Collaborative innovation center of chemical science and Engineering Tianjin 300072

Multidimensional mechanical flexible organic crystals with tunable optoelectronic properties hold significant promise for practical application in complicated environmental ***,based on a newly designed“flexible”Schiff base small molecule with chirality,we presented a compatibly bendable and twistable organic single crystal with circularly polarized luminescence for the first ***,the twodimensional elastic bending of the chiral crystal was realized at both room and liquid nitrogen temperatures,along with recoverable plastic twisting at room ***,circular dichroism and circularly polarized luminescence spectroscopy were employed to characterize the chiral enantiomer in solution and the solid *** design strategy provides a new perspective for the future construction of chiroptical flexible crystal materials.

关键词： organic crystal multidimensional flexibility circularly polarized luminescence low-temperature resistance