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Phthalocyanine-derived catalysts decorated by metallic nanoclusters for enhanced CO_(2)electroreduction

Green Energy & Environment 2023年第2期8卷 444-451页

作者： Jiacheng Chen Jiayu Li Jing Xu Minghui Zhu Yi-Fan Han State Key Laboratory of Chemical Engineering School of Chemical EngineeringEast China University of Science and TechnologyShanghai200237China

Electrochemical CO_(2)reduction(CO_(2)RR)over molecular catalysts is a paramount approach for CO_(2)conversion to ***,we report a novel phthalocyanine-derived catalyst synthesized by a two-step method with a much improved ***,the catalyst contains both Ni-N4sites and highly dispersed metallic Ni nanoclusters,leading to an increased CO_(2)RR currents by two *** labelling study and in situ spectroscopic analysis demonstrate that the existence of metallic Ni nanoclusters is the key factor for the activity enhancement and can shift the CO_(2)RR mechanism from being electron transfer(ET)-limited(forming*COO^(-))to concerted proton-electron transfer(CPET)-limited(forming CO).

关键词： Carbon dioxide Electroreduction Hybrid catalyst Nickel-based catalysts Mechanism

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Deactivation and regeneration of the commercial Cu/ZnO/Al_(2)O_(3) catalyst in low-temperature methanol steam reforming

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Science China Chemistry 2023年第12期66卷 3645-3652页

作者： Didi Li Zhen Wang Shiqing Jin Minghui Zhu State Key Laboratory of Chemical Engineering School of Chemical EngineeringEast China University of Science and TechnologyShanghai 200237China

Cu-based catalysts with excellent activity at low temperatures are widely used for methanol steam reforming(MSR)but suffer from deactivation *** present work aims to elucidate the deactivation and regeneration mechanisms of the commercial Cu/ZnO/Al_(2)O_(3) catalyst in low temperature *** employing a series of(quasi)in situ characterization methods,it is found that the deactivation of the catalyst at a high weight hourly space velocity(WHSV)and a low reaction temperature is mainly due to the poisoning of Cu species associated with surface-oxygenated species with less Cu sintering,rather than carbon deposition,and strong metal-support interaction(SMSI).An in situ regeneration method was developed for the deactivated commercial Cu/ZnO/Al_(2)O_(3) catalyst via the simultaneous supply of O_(2).It is shown that the addition of O_(2)(≥1 vol%)can reverse the deactivation caused by surface-oxygenated poisoning due to the weak interaction between formed surface copper oxide and surface-oxygenated species,facilitating their desorption,but not deactivation caused by sintering,thereby partially restoring the catalytic activity.

关键词： methanol steam reforming Cu/ZnO/Al_(2)O_(3)catalyst deactivation regeneration

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Kinetics and mechanistic insights into the active sites of Au catalysts for selective propylene oxidation

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Nano Research 2023年第5期16卷 6220-6227页

作者： Qianhong Wang Zhihua Zhang Keng Sang Wenyao Chen Gang Qian Jing Zhang Xinggui Zhou Xuezhi Duan State Key Laboratory of Chemical Engineering School of Chemical EngineeringEast China University of Science and TechnologyShanghai 200237China

Identification of the catalytically active sites emerges as the prerequisite for an atomic-level comprehensive understanding and further rational design of highly efficient ***,we demonstrate a kinetics strategy to identify the active sites of Au catalyst for the disentanglement of geometric and electronic effects on the selective oxidation of propylene to *** the Ti-containing titanium-silicalite-1(TS-1)and Ti-free silicalite-1(S-1)were employed as supports to immobilize Au catalysts,which were investigated by a combination of multiple characterization,kinetics analysis,crystal structure *** Au(111)sites are identified as the main active site for acrolein formation,while their electronic effects are highly relevant to the presence or absence of ***,propylene epoxide(PO)formation mainly involves the co-participation of Au and Ti sites,the proximity between Au and Ti sites is found to have less influences on PO formation in a certain *** comparison,acrolein is very likely to generate over Au(111)sites via the hydrogen-assisted O_(2) activation to oxygenated species for its oxidizing *** insights gained here could guide the design and preparation of Au catalysts for selective propylene oxidation.

关键词： propylene oxidation Au catalysts active site geometric and electronic effects Au-Ti proximity

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Amorphous hybrid tungsten oxide–nickel hydroxide nanosheets used as a highly efficient electrocatalyst for hydrogen evolution reaction

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Nano Research 2024年第4期17卷 2499-2508页

作者： Chao Lyu Chenghai Dai Yiwei Tan State Key Laboratory of Materials-Oriented Chemical Engineering School of Chemistry and Chemical EngineeringNanjing Tech UniversityNanjing 211816China

There are more challenges for alkaline hydrogen evolution reaction(HER)via simultaneously expediting the electron-coupled water dissociation process(Volmer step)and the following electrochemical H_(2) desorption(Heyrovsky step).Hybrid amorphous electrocatalysts are highly desirable for efficient hydrogen evolution from water-alkali electrolyzers due to the bifunctionality for the different elementary steps of HER and optimal interactions with water molecules and the reactive hydrogen intermediates(Had).Herein,the synthesis of amorphous hybrid ultrathin(tungsten oxide/nickel hydroxide)hydrate(a-[WO_(3)/Ni(OH)_(2)]·0.2H_(2)O)nanosheets on nickel foam(NF)for efficient alkaline HER is *** structural and composition features of a-[WO_(3)/Ni(OH)_(2)]·0.2H_(2)O are characterized in *** resulting a-[WO_(3)/Ni(OH)_(2)]·0.2H_(2)O/NF electrocatalyst with the synergistic effect of both hybrid components for the HER elementary steps shows greatly improved the activity and durability for the HER with a low overpotential of-41 and-163 mV at-10 and-500 mA·cm^(-2),respectively,a Tafel slope as low as-72.9 mV·dec^(-1),and long-term stability of continuous electrolysis for at least 150 h accompanying by inappreciable overpotential change in 1 M *** the hybrid a-[WO_(3)/Ni(OH)_(2)]·0.2H_(2)O,Ni(OH)_(2) and WO_(3) moieties are separately responsible for accelerating dissociative adsorption of water and weakening Had adsorption strength,which is beneficial to the improvement of the alkaline HER activity.

关键词： amorphous nanomaterial bimetallic electrocatalyst tungsten oxide ultrathin nanosheet hydrogen evolution reaction

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Polybenzoxazine/organosilicon composites with low dielectric constant and dielectric loss

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Chinese Journal of chemical engineering 2023年第12期64卷 241-249页

作者： Manlin Yuan Xin Lu Xiaoyun Ma Hao Lin Angui Lu Liyan Shao Zhong Xin State Key Laboratory of Chemical Engineering School of Chemical EngineeringEast China University of Science and TechnologyShanghai 200237China

The evolution of electronic communication technology raises higher requirements for low dielectric constant(low-k)*** this,a benzoxazine functional organosilicon(HP-aptes)with dense Si—O—Si crosslinking networks and large sterically hindered tert-butyl groups was prepared by the sol–gel ***,a series of polybenzoxazine composites(PPHP)were prepared from intrinsically low dielectric constant bis-functional benzoxazine monomer(P-aptmds)and *** double crosslinking networks of polybenzoxazine and organosilicon further increased the crosslinking density and decreased the dipole density of composites,which endowed the composites with enhanced low-k *** the content of HP-aptes is 30%(mass),the crosslinking density was 2.05×10^(-3)mol·cm^(-3),while that of PP-aptmds was 3.31×10^(-3)mol·cm^(-3).In addition,the dielectric constant and dielectric loss of PPHP composite at 1 MHz could reach 2.61 and 0.0056,respectively.

关键词： Polybenzoxazine Organosilicon Composite Dielectric constant

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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

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Effect of solvent on the initiation mechanism of living anionic polymerization of styrene:A computational study

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Chinese Journal of chemical engineering 2024年第5期69卷 135-142页

作者： Shen Li Yin-Ning Zhou Zhong-Xin Liu Zheng-Hong Luo School of Chemical Engineering and Technology Hainan UniversityHaikou 570228China Department of Chemical Engineering School of Chemistry and Chemical EngineeringState Key Laboratory of Metal Matrix CompositesShanghai Jiao Tong UniversityShanghai 200240China

For living anionic polymerization(LAP),solvent has a great influence on both reaction mechanism and *** this work,by using the classical butyl lithium-styrene polymerization as a model system,the effect of solvent on the mechanism and kinetics of LAP was revealed through a strategy combining density functional theory(DFT)calculations and kinetic *** terms of mechanism,it is found that the stronger the solvent polarity,the more electrons transfer from initiator to solvent through detailed energy decomposition analysis of electrostatic interactions between initiator and solvent ***,we also found that the stronger the solvent polarity,the higher the monomer initiation energy barrier and the smaller the initiation rate ***,initiation is more favorable at lower temperatures based on the calculated results ofΔG_(TS).Finally,the kinetic characteristics in different solvents were further examined by kinetic *** is found that in benzene and n-pentane,the polymerization rate exhibits first-order ***,slow initiation and fast propagation were observed in tetrahydrofuran(THF)due to the slow free ion formation rate,leading to a deviation from first-order kinetics.

关键词： Living anionic polymerization Solvent effect Reaction kinetics Computational chemistry Mathematical modeling Kinetic modeling

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Multi-channel photogenerated charge transfer in double S-scheme for promoting photostability and mineralization of pollutants

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Journal of Materials Science & technology 2024年第35期202卷 67-81页

作者： Runlin Chen Lifeng Li Yufeng Gong Hongming Lou Yuxia Pang Dongjie Yang Xueqing Qiu School of Chemistry and Chemical Engineering Guangdong Provincial Key Lab of Green Chemical Product TechnologyState Key Laboratory of Pulp and Paper EngineeringSouth China University of TechnologyGuangzhou 510640China School of Chemical Engineering and Light Industry Guangdong University of TechnologyGuangzhou 510006China

Superior photo-mineralization of pollutants,outstanding charge separation efficiency and exceptional photostability of catalysts constitute three pivotal factors for the effective photodegradation of organic *** this study,a dual S-scheme In2 O3/Pedot/In2 S3(IO/Pedot/IS),inspired by natural photosyn-thesis,was successfully synthesized for the degradation of lignin and *** resulting exceptional semiconductor contact creates a dual-interface electric field on Pedot,facilitating multi-channel charge transport and enhancing charge separation *** establishment of the dual S-scheme hetero-junction raised the reduction-oxidation potential of the type-II In2 O3/In2 *** subjected to 5 W LED irradiation for 60 min,IO/Pedot-2/IS demonstrated a remarkable mineralization rate of 85.8%for sodium lignosulfonate(SL),surpassing the 53.7%mineralization rate achieved by IO/***,the degra-dation efficiency for tetracycline(TC)and ciprofloxacin(CIP)reached 91%and 88%,***,the hole(h+)conductivity of Pedot efficiently alleviated the photocorrosion of sulfide,ensuring robust cyclic *** simulations of natural photocatalysis showcased the exceptional versatility and applicability of IO/Pedot/***-depth analysis led to the proposal of a potential photodegradation pathway for lignin,based on the intermediates detected through liquid chromatography-mass spectrom-etry(LC-MS).Overall,this study presents an effective strategy for the efficient photocatalytic treatment of organic pollutants.

关键词： Photodegradation Lignin Pedot Photocorrosion Double S-scheme

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Highly selective electrosynthesis of 3,4-dihydroisoquinoline accompanied with hydrogen production over three-dimensional hollow CoNi-based microarray electrocatalysts

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Nano Research 2024年第4期17卷 2509-2519页

作者： Yu Xin Liyu Chen Yingwei Li Kui Shen Guangdong Provincial Key Lab for Green Chemical Product Technology School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510640China State Key Laboratory of Pulp and Paper Engineering School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510640China

Electrocatalytic oxidation reaction of biomass-based derivatives is an excellent candidate to replace water oxidation for obtaining both value-added products and hydrogen(H_(2)),but the exploration of competent electrocatalysts is still highly ***,two new types of three-dimensional self-supported hollow microarrays containing CoNi layered double hydroxide(CoNi-LDH)and N-doped carbon nanosheets decorated with CoNi alloyed nanoparticles(CoNi-NC)on carbon cloth(CC)are prepared,which are further used as efficient electrocatalysts for tetrahydroisoquinoline(THIQ)electrooxidation and hydrogen evolution reaction(HER),*** demonstrate that the Co-modulated electronic environment for Ni(II)/Ni(Ⅲ)redox-looping in CoNi-LDH is the main factor to boost the selectivity of 3,4-dihydroisoquinoline(DHIQ)for the indirect electrooxidation process of *** functional theory(DFT)calculations reveal that the Ni(Ⅲ)/Co(Ⅲ)dual sites of CoNi-LDH exhibit enhanced adsorption for THIQ but poorer adsorption for DHIQ compared to pure Co(Ⅲ)or Ni(Ⅲ).Therefore,the Ni(Ⅲ)/Co(Ⅲ)dual sites can effectively inhibit the peroxidation of DHIQ to isoquinoline(IQ)over CoNi-LDH,thus improving the selectivity of DHIQ to nearly 100%,much higher than that of its pure Ni ***,CC@CoNi-NC can deliver high HER activity with low overpotential(40 mV@10 mA·cm^(-2))and high exchange current density(3.08 mA·cm^(-2)).Impressively,the assembled flow-cell device with CC@CoNi-LDH anode and CC@CoNi-NC cathode only requires low cell voltage and electricity consumption of 1.6 V and 3.50 kWh per cubic meter of H_(2)(@25 mA·cm^(-2)).

关键词： highly selective electrosynthesis dihydroisoquinolines hydrogen evolution reaction metal-organic frameworks hollow microarrays

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Highly Conductive Proton Selectivity Membrane Enabled by Hollow Carbon Sieving Nanospheres for Energy Storage Devices

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engineering 2023年第9期28卷 69-78页

作者： Kang Huang Shuhao Lin Yu Xia Yongsheng Xia Feiyan Mu Yuqin Lu Hongyan Cao Yixing Wang Weihong Xing Zhi Xu State Key Laboratory of Materials-Oriented Chemical Engineering College of Chemical EngineeringNanjing Tech UniversityNanjing 211816China State Key Laboratory of Chemical Engineering School of Chemical EngineeringEast China University of Science and TechnologyShanghai 200237China

Ion conductive membranes(ICMs)with highly conductive proton selectivity are of significant importance and greatly desired for energy storage ***,it is extremely challenging to construct fast proton-selective transport channels in ***,a membrane with highly conductive proton selectivity was fabricated by incorporating porous carbon sieving nanospheres with a hollow structure(HCSNs)in a polymer *** to the precise ion sieving ability of the microporous carbon shells and the fast proton transport through their accessible internal cavities,this advanced membrane presented a proton conductivity(0.084 S·cm^(-1))superior to those of a commercial Nation 212(N212)membrane(0.033S·cm^(-1))and a pure polymer membrane(0.049 S·cm^(-1)).The corresponding proton selectivity of the membrane(6.68×10^(5) S·min·cm^(-3))was found to be enhanced by about 5.9-fold and 4.3-fold,respectively,compared with those of the N212 membrane(1.13×10^(5) S·min·cm^(-3))and the pure membrane(1.56×10^(5) S·min·cm^(-3)).Low-field nuclear magnetic resonance(LF-NMR)clearly revealed the fast protonselective transport channels enabled by the HCSNs in the polymeric *** proposed membrane exhibited an outstanding energy efficiency(EE)of 84%and long-term stability over 1400 cycles with a0.065%capacity decay per cycle at 120 mA·cm^(-2) in a typical vanadium flow battery(VFB)system.

关键词： Ion conductive membrane Hollow carbon sieving nanosphere Proton transport channel Flow battery

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