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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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Confinement of ionomer for electrocatalytic CO2 reduction reaction via efficient mass transfer pathways

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National Science Review 2024年第2期11卷 168-176页

作者： Xiaowei Du Peng Zhang Gong Zhang Hui Gao Lili Zhang Mengmeng Zhang Tuo Wang Jinlong Gong school of chemical Engineering and Technology Key Laboratory for Green Chemical Technology of the Ministry of Education Tianjin University Collaborative Innovation Center of chemical Science and Engineering(Tianjin) National Industry-Education Platform of Energy Storage Tianjin University Joint school of the National University of Singapore and Tianjin University International Campus of Tianjin University Haihe Laboratory of Sustainable chemical Transformations

Gas diffusion electrodes（GDEs） mediate the transport of reactants, products and electrons for the electrocatalytic CO2reduction reaction（CO2RR） in membrane electrode assemblies. The random distribution of ionomer, added by the traditional physical mixing method, in the catalyst layer of GDEs affects the transport of ions and CO2. Such a phenomenon results in elevated cell voltage and decaying selectivity at high current densities. This paper describes a pre-confinement method to construct GDEs with homogeneously distributed ionomer, which enhances mass transfer locally at the active centers. The optimized GDE exhibited comparatively low cell voltages and high CO Faradaic efficiencies（FE > 90%） at a wide range of current densities. It can also operate stably for over 220 h with the cell voltage staying almost unchanged. This good performance can be preserved even with diluted CO2feeds, which is essential for pursuing a high single-pass conversion rate. This study provides a new approach to building efficient mass transfer pathways for ions and reactants in GDEs to promote the electrocatalytic CO2RR for practical applications.

关键词： CO2 electroreduction gas diffusion electrode mass transfer ionomer Ag catalyst

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Piezoelectric-enhanced n-TiO2/BaTiO3/p-TiO2 heterojunction for highly efficient photoelectrocatalysis

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Green Energy & Environment 2024年第9期9卷 1466-1476页

作者： Minhua Ai Zihang Peng Xidi Li Faryal Idrees Xiangwen Zhang Ji-Jun Zou Lun Pan Key Laboratory for Green chemical Technology of the Ministry of Education School of Chemical Engineering and Technology Tianjin University Collaborative Innovative Center of chemical Science and Engineering (Tianjin) Haihe Laboratory of Sustainable chemical Transformations Department of Physics University of the Punjab Quaid-e-Azam Campus

Charge separation is critical for achieving efficient solar-to-hydrogen conversion,whereas piezoelectric-enhanced photoelectrochemical（PEC） systems can effectively modulate band bending and charge ***,we design an n-Ti O2/Ba Ti O3/p-Ti O2（TBTm） heterojunction in which the piezoelectric Ba Ti O3layer is sandwiched between n-Ti O2and p-Ti *** built-in electric field of TBTm can provide a strong driving force to accelerate carrier separation and prolong carrier ***,the TBT3 achieves a prominent photocurrent density,as high as 2.13 m A cm-2at 1.23 V versus reversible hydrogen electrode （RHE）,which is 2.4-and 1.5-times higher than Ti O2and Ti O2–Ba Ti O3heterojunction,*** by mechanical deformation,the induced dipole polarization can further regulate built-in electric fields,and the piezoelectric photocurrent density of TBT3-800 is 2.84 times higher than Ti O2at 1.23 V *** due to the construction of *** work provides a piezoelectric polarization strategy for modulating the built-in electric field of heterojunction for PEC system.

关键词： Photoelectrochemical Piezoelectric polarization Heterojunction Charge separation

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Effects of orientation on the fatigue crack growth behaviors of the ZK60 magnesium alloy in air and PBS

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Journal of Magnesium and Alloys 2024年第1期12卷 281-294页

作者： Jiaqi Hu Zheng Liu Zuoliang Ning Hong Gao school of chemical Engineering and Technology Tianjin UniversityTianjin 300072China Tianjin Key Laboratory of chemical Process Safety and Equipment Technology Tianjin 300072China

Strong anisotropic corrosion and mechanical properties caused by specimen orientations greatly limit the applications of wrought magnesium *** investigate the influences of specimen orientation,the corrosion tests and(corrosion)fatigue crack growth tests were *** rolled and transverse surfaces of the materials show distinct corrosion rate differences in the stable corrosion stage,but the truth is the opposite for the initial stage of *** air,specimen orientations have a significant influence on the plastic deformation mechanisms near the crack tip,which results in different fatigue fracture surfaces and cracking *** with R-T specimens,N-T specimens show a slower fatigue crack growth(FCG)rate in air,which can be attributed to crack closure effects and deformation twinning near the crack *** corrosion environment will not significantly change the main plastic deformation mechanisms for the same type of ***,the FCG rate in phosphate buffer saline(PBS)is one order of magnitude higher than that in air,which is caused by the combined effects of hydrogen-induced cracking and anodic *** to the similar corrosion rates at crack tips,the specimens with different orientations display close FCG rates in PBS.

关键词： Magnesium alloy Orientation Corrosion Fatigue crack growth

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Controllable CPL response driven by achiral UV-photosensitive dichroic dye through cholesteric liquid crystals

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Science China Chemistry 2024年第4期67卷 1250-1255页

作者： Yihan Chen Yang Li Hang Li Lulu Li Yiwu Quan Yixiang Cheng State Key Laboratory of Analytical Chemistry for Life Science School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China Key Laboratory of High-Performance Polymer Material and Technology of Ministry of Education School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China school of Environmental and chemical Engineering Jiangsu University of Science and TechnologyZhenjiang 212003China

Versatile stimuli-responsive circularly polarized luminescent(CPL)materials have potential applications in information storage,security encryption,and intelligent *** this study,the Z/E isomerization of ultraviolet(UV)-photosensitive achiralα-cyanostilbene derivative was used as an achiral dichroic dye(Switch)to drive the controllable CPL-active response in cholesteric liquid crystals(CLCs).Under irradiation by 365 nm UV light,the resulting CLCs-Z-Switch underwent a Z-to-E configuration isomerization as CLCs-E-Switch,accompanied by a decrease in its dichroic order parameter(SFvalue)from 0.15to *** the quantum yield(QY)of CLCs-E-Switch increased from 8.1%(CLCs-Z-Switch)to 16.8%,the corresponding glumvalues of CPL emission decreased from+0.55/-0.57 to+0.37/-0.39 due to a decrease in the order of helical arrangement of E-Switch in E7 *** study enables photosensitive CLCs-Switch to be applied for optical information storage devices.

关键词： circularly polarized luminescent photosensitive dichroic dye cholesteric liquid crystals chiral induction

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Electrode/Electrolyte Interfacial Chemistry Modulated by Chelating Effect for High-Performance Zinc Anode

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Energy & Environmental Materials 2024年第3期7卷 93-99页

作者： Chuanlin Li Guangmeng Qu Xixi Zhang Chenggang Wang Xijin Xu school of Physics and Technology University of JinanJinan 250022China school of Chemistry and chemical Engineering Shandong UniversityJinan 250100China

Although Zn metal has been regarded as the most promising anode for aqueous batteries,its practical application is still restricted by side reactions and dendrite ***,an in-situ solid electrolyte interphase(SEI)film formed on the interface of electrode/electrolyte during the plating/stripping of zinc anodes by introducing trace amounts of multidentate ligand sodium diethyldithiocarbamate(DDTC)additive into 1 M ZnSO_(4).The synergistic effect of in-situ solid electrolyte interphase forming and chelate effect endows Zn^(2+)with uniform and rapid interface-diffusion kinetics against dendrite growth and surface side *** a result,the Zn anode in 1 M ZnSO_(4)+DDTC electrolytes displays an ultra-high coulombic efficiency of 99.5%and cycling stability(more than 2000 h),especially at high current density(more than 600 cycles at 40 mA cm^(-2)).Moreover,the Zn//MnO_(2)full cells in the ZnSO_(4)+DDTC electrolyte exhibit outstanding cyclic stability(with 98.6%capacity retention after 2000 cycles at 10 C).This electrode/electrolyte interfacial chemistry modulated strategy provides new insight into enhancing zinc anode stability for high-performance aqueous zinc batteries.

关键词： chelating effect in-situ SEI ultra-high current density Zn anodes

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NaBH4-induced phase transition of CoSe_(2) with abundant Se deficiency for acidic oxygen reduction to hydrogen peroxide

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Rare Metals 2024年第2期43卷 500-510页

作者： Cai-Di Han Yong-Chao Zhang Qian Zhang Jin-Ting Wu Jian Gao Ji-Jun Zou Xiao-Dong Zhu State Key Laboratory Base of Eco-chemical Engineering College of chemical Engineering Qingdao University of Science and TechnologyQingdao266042China Key Laboratory for Green chemical Technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin300072China

Electrocatalytic oxygen reduction(ORR)via the 2e−pathway to form H_(2)O_(2) in acidic medium has attracted extensive ***,the low activity,insufficient selectivity and high cost of catalysts have been the ***,CoSe_(2) with abundant Se deficiency was synthesized by a simple hydrothermal method,and the addition of NaBH4-induced CoSe_(2) phase transition from orthorhombic to cubic phase with more Se *** cubic phase CoSe_(2) with abundant Se deficiency can effectively regulate the surface electronic structure with suitable binding energies of*OOH and*O,which shows high activity,selectivity and long-term stability for acidic ORR to H_(2)O_(2).The onset potential is as low as 0.73 V *** hydrogen electrode(RHE),the H_(2)O_(2) selectivity is 84%(0 V ***),and the average electron transfer number is about ***,the H_(2)O_(2) yield measured using a flow cell is as high as 115.92 mmol·gcat.^(−1)·h^(−1) and the Faradaic efficiency is 70%at 0 V ***,which presents high potential in electrocatalytic acidic ORR to H_(2)O_(2) and organic pollutant degradation using the electron-Fenton process.

关键词： Se defected CoSe_(2) Crystal phase transition Electrocatalysis Acidic oxygen reduction Hydrogen peroxide

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One-step growth of ultrathin CoSe_(2)nanobelts on N-doped MXene nanosheets for dendrite-inhibited and kinetic-accelerated lithium-sulfur chemistry

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Science Bulletin 2024年第13期69卷 2059-2070页

作者： Chuanliang Wei Zhengran Wang Peng Wang Xinlu Zhang Xuguang An Jinkui Feng Baojuan Xi Shenglin Xiong school of Chemistry and chemical Engineering School of Materials Science and EngineeringShandong UniversityJinan 250100China school of Mechanical Engineering Chengdu UniversityChengdu 610106China

The practical application of lithium–sulfur(Li–S)batteries is inhibited by the shuttle effect of lithium polysulfides(LiPSs)and slow polysulfide redox kinetics on the S cathode as well as the uncontrollable growth of dendrites on the Li metal ***,both cathode and anode sides must be considered when modifying LiS ***,two-dimensional(2D)ultrathin CoSe_(2)nanobelts are in situ grown on 2D N-doped MXene nanosheets(CoSe_(2)@N-MXene)via one-step solvothermal process for the first *** to its unique 2D/2D structure,CoSe_(2)@N-MXene can be processed to crumpled nanosheets by freeze-drying and flexible and freestanding films by vacuum *** crumpled CoSe_(2)@NMXene nanosheets with abundant active sites and inner spaces can act as S hosts to accelerate polysulfide redox kinetics and suppress the shuttle effect of LiPSs owing to their strong adsorption ability and catalytic conversion effect with ***,the CoSe_(2)@N-MXene film(CoSe_(2)@NMF)can act as a current collector to promote uniform Li deposition because it contains lithiophilic CoSe_(2)and N *** the systematic effect of CoSe_(2)@N-MXene on S cathode and Li metal anode,the electrochemical and safety performance of Li–S batteries are ***_(2)@NMF also shows excellent storage performances in flexible energy storage devices.

关键词： Ultrathin CoSe_(2)nanobelts N-doped MXene nanosheets In situ growth Flexible MXene-based films Li-S batteries

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An unexpected approach to enhance specific surface area and mesopore amount of polyaniline by Zn doping

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Rare Metals 2024年第9期43卷 4585-4594页

作者： Zhi-Da Zhu Yu-Zhe Han Xiao-Bi Jing school of Mechanical Engineering Yangzhou UniversityYangzhou 225127China school of Chemistry and chemical Engineering Yangzhou UniversityYangzhou 225002China

Poly-p-anisidine could be easily fabricated via the oxidative polymerization reaction of p-anisidine using H_(2)O_(2)as the green *** was unexpectedly found that zinc doping could significantly improve the adsorption ability of the material versus heavy metals such as Pb,Cu,Pd,Ag and *** of nitrogen adsorption–desorption experiments demonstrated that Zn doping could enhance the specific surface area and mesopore amount of the prepared material,which might facilitate its absorption to *** work not only provides a novel material for the treatment of heavy metal-polluted water but also leads to a nice mesoporous catalyst support for environment protection and organic synthesis,*** Zn-doped poly-panisidine can be employed as the catalyst support to prepare Cu@PANI-OMe/Zn or Pd@PANI-OMe/Zn for the oxidative degradation reaction of phenol or Suzuki–Miyaura coupling reactions,*** discloses a new strategy for fabricating the mesoporous polyaniline materials with profound application potential.

关键词： Surfaces Porous materials Rare metal concentration Adsorption Catalysis

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Strong metal-support interaction between AuPd nanoparticles and oxygen-rich defect ZrO_(2) for enhanced catalytic 5-hydroxymethylfurfural oxidation

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Chinese chemical Letters 2024年第2期35卷 507-511页

作者： Yunlei Zhang Yiran Liu Wen Guan Mengxue Cao Yao Chen Pengwei Huo Institute of Green Chemistry and chemical Technology School of Chemistry and Chemical EngineeringJiangsu UniversityZhenjiang 212013China school of the Environment and Safety Jiangsu UniversityZhenjiang 212013China

The unique properties of metal oxide surfaces,crystal surfaces and defects play vital roles in biomass upgrading *** this work,hierarchical porous bowl-shaped ZrO_(2)(HB-ZrO_(2))with mixed crystal phase was designed and employed as the support for loading AuPd bimetal with different proportions to synthesize AuPd/HB-ZrO_(2) *** effects of surface chemistry,oxygen defects,bimetal interaction and metal-support interaction of AuPd/HB-ZrO_(2) on catalytic performance for the selective oxidation of 5-hydroxymethylfurfural(HMF)to 2,5-furandicarboxylic acid(FDCA)were systematically *** Au 2 Pd1/HB-ZrO_(2) catalyst afforded a satisfactory FDCA yield of 99.9%from HMF oxidation using O_(2) as the oxidant in water,accompanied with an excellent FDCA productivity at 97.6 mmol g^(−1) h^(−1).This work offers fresh insights into rationally designing efficient catalysts with oxygen-rich defects for the catalytic upgrading of biomass platform chemicals.

关键词： 5-Hydroxymethylfurfural oxidation 2,5-Furandicarboxylic acid Oxygen-rich defect ZrO_(2) AuPd bimetal Bowl-shaped structure

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