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Chinese Journal of chemical Engineering 2024年第4期68卷 83-93页

作者： Zhihao Yang Li Chen Jian Xue Miaomiao Su Fangdan Zhang Liangxin Ding Suqing Wang Haihui Wang guangdong provincial key lab of green chemical product technology School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510640China Beijing key laboratory of Membrane Materials and Engineering Department of Chemical EngineeringTsinghua UniversityBeijing 100084China

Separators play a critical role in the safety and performance of lithium-ion ***,commercial polyolefin separators are limited by their poor affinity with electrolytes and low melting *** this work,we constructed a reinforced-concrete-like structure by homogeneously dispersing nano-Al_(2)O_(3) and cellulose on the separators to improve their stability and *** this reinforcedconcrete-like structure,the cellulose is a reinforcing mesh,and the nano-Al_(2)O_(3) acts as concrete to support the *** constructing the reinforced-concrete-like structure,the separators exhibit good stability even at 200℃(thermal shrinkage of 0.3%),enhanced tensile strain(tensile stress of 133.4 MPa and tensile strains of 62%),and better electrolyte wettability(a contact angle of 6.5°).Combining these advantages,the cells with nano-Al_(2)O_(3)@cellulose-coated separators exhibit stable cycling performance and good rate ***,the construction of the reinforced-concretelike structure is a promising technology to promote the application of lithium-ion batteries in extreme environments.

关键词： Alumina Nanomaterials Lithium-ion batteries Membranes Cellulose Reinforced-concrete-like structure

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

Role of methoxy and C_(α)-based substituents in electrochemical oxidation mechanisms and bond cleavage selectivity of β-O-4 lignin model compounds

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green Energy & Environment 2024年第1期9卷 114-125页

作者： Yang Zhou Qiang Zeng Hongyan He Kejia Wu Fuqiao Liu Xuehui Li School of Chemistry and chemical Engineering The Guangdong Provincial Key Laboratory of Green Chemical Product TechnologyState Key Laboratory of Pulp and Paper EngineeringSouth China University of TechnologyGuangzhouGuangdong510640China CAS key laboratory of green Process and Engineering Institute of Process EngineeringChinese Academy of SciencesBeijing100190China

In order to better understand the specific substituent effects on the electrochemical oxidation process of β-O-4 bond, a series of methoxyphenyl type β-O-4 dimer model compounds with different localized methoxyl groups, including 2-(2-methoxyphenoxy)-1-phenylethanone, 2-(2-methoxyphenoxy)-1-phenylethanol, 2-(2-methoxyphenoxy)-1-(4-methoxyphenyl)ethanone, 2-(2-methoxyphenoxy)-1-(4-methoxyphenyl)ethanol, 2-(2,6-dimethoxyphenoxy)-1-(4-methoxyphenyl)ethanone, 2-(2,6-dimethoxyphenoxy)-1-(4-methoxyphenyl)ethanol have been selected and their electrochemical properties have been studied experimentally by cyclic voltammetry, and FT-IR spectroelectrochemistry. Combining with electrolysis products distribution analysis and density functional theory calculations, oxidation mechanisms of all six model dimers have been explored. In particular, a total effect from substituents of both para-methoxy(on the aryl ring closing to Cα) and Cα-OH on the oxidation mechanisms has been clearly observed, showing a significant selectivity on the Cα-Cβbond cleavage induced by electrochemical oxidations.

关键词： Lignin model compounds β-O-4 dimers Electrochemical oxidation Oxidation mechanisms Substituent effect

Recycling of waste aluminum scraps to fabricate sulfidated zero-valent iron-aluminum particles for enhanced chromate removal

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Journal of Environmental Sciences 2024年第4期138卷 650-659页

作者： Yahui Zhang Liguo Zhang Jiajia Zeng Shuqun Xu Jianyu Pan Wenzhuo Huang Jianliang Sun Feng Jiang guangdong provincial key laboratory of chemical Pollution and Environmental Safety&MOE key laboratory of Theoretical Chemistry of Environment School of EnvironmentSouth China Normal UniversityGuangzhou 510006China guangdong provincial key lab of Environmental Pollution Control and Remediation technology School of Environmental Science&EngineeringSun Yat-Sen UniversityGuangzhou 510275China

Massive waste aluminum scraps produced from the spent aluminum products have high electron capacity and can be recycled as an attractive alternative to materials based on zerovalent iron(Fe^(0))for the removal of oxidative contaminants from *** study thus proposed an approach to fabricate micron-sized sulfidated zero-valent iron-aluminum particles(S-Al^(0)@Fe^(0))with high reactivity,electron selectivity and capacity using recycled waste aluminum scraps.S-Al^(0)@Fe^(0)with a three-layer structure contained zero-valent aluminum(Al^(0))core,Fe^(0) middle layer and iron sulfide(FeS)*** rates of chromate(Cr(Ⅵ))removal by S-Al^(0)@Fe^(0)at pH 5.0-9.0 were 1.6-5.9 times greater than that by sulfidated zero-valent iron(S-Fe^(0)).The Cr(Ⅵ)removal capacity of S-Al^(0)@Fe^(0)was 8.2-,11.3-and 46.9-fold greater than those of S-Fe0,zero-valent iron-aluminum(Al^(0)-Fe^(0))and Fe^(0),*** chemical cost of S-Al^(0)@Fe^(0) for the equivalent Cr(Ⅵ)removal was 78.5%lower than that of S-Fe^(0).Negligible release of soluble aluminum during the Cr(Ⅵ)removal was *** significant enhancement in the reactivity and capacity of S-Al^(0)@Fe^(0)was partially ascribed to the higher reactivity and electron density of the Al0core than Fe^(0).More importantly,S-Al^(0)@Fe^(0) served as an electric cell to harness the persistent and selective electron transfer from the Al^(0)-Fe^(0) core to Cr(Ⅵ)at the surface via coupling Fe^(0)-Fe^(2+)-Fe^(3+)redox cycles,resulting in a higher electron utilization ***,S-Al^(0)@Fe^(0) fabricated using recycled waste aluminum scraps can be a cost-effective and environmentally-friendly alternative to S-Fe^(0) for the enhanced removal of oxidative contaminants in industrial wastewater.

关键词： Recycled waste aluminum scraps Oxidative contaminants Cr(Ⅵ)reduction Sulfidated Al^(0)@Fe^(0)particle Electron transfer

Bimetallic NiCoP catalysts anchored on phosphorus-doped lignin-based carbon for robust oxygen evolution performance

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Rare Metals 2024年第7期43卷 3084-3095页

作者： Ling-Ying-Zi Xiong Bo-Wen Liu Lei Du Yue-Kuan Zhou Xu-Liang Lin Huan Wang guangdong Engineering technology Research Center for Sensing Materials & Devices Guangzhou Key Laboratory of Sensing Materials & DevicesSchool of Chemistry and Chemical EngineeringGuangzhou University School of chemical Engineering and Light Industry Guangdong University of Technology guangdong provincial laboratory of Chemistry and Fine chemical Engineering Jieyang Center Sustainable Energy and Environment Thrust Function HubThe Hong Kong University of Science and Technology (Guangzhou) Division of Emerging Interdisciplinary Areas Department of Mechanical and Aerospace EngineeringThe Hong Kong University of Science and Technology State key lab of Pulp and Paper Engineering South China University of Technology

Oxygen evolution reaction（OER） catalysts are the key core materials that determine the performance of fuel cells,metal-air batteries,electrolytic water decomposition,and other *** this work,a green lignin-based non-precious metal OER catalyst was prepared by a simple ***,c arboxylated lignin was used to complex Ni and Co in situ,and then they were placed with sodium hypophosphite in the same tube furnace for upstream and downstream high-temperature calcination to construct a lignin carbon-based Ni-Co bimetallic OER catalyst（NiCoP@C）.The synthesized catalyst is a porous bimetallic phosphide with a three-dimensional network structure and high-density electrochemical active ***@C exhibited favorable catalytic activity for the oxygen evolution reaction（OER） with overpotential of 280 mV at 10 mA·cm-2and a Tafel slope of 77 mV·***,it exhibited remarkable durability during *** functional theory（DFT） calculations revealed that by leveraging the distinctive structure of transition metal phosphide nanoparticles incorporated into a reticulated substrate,the NiCoP@C catalyst offered an increased number of active sites for OER catalysis,significantly enhancing its stability during practical *** present study broadens the utilization pathways of biomass to "turn waste into treasure," aligning the development concept of green sustainable development.

关键词： Oxygen evolution reaction Lignin Carbon-based catalyst Nickel–cobalt bimetal Metal phosphide

Direct synthesis of a disinfectant with fresh scent of green plants by semi-hydrogenation of alkynol on Pd single-atom catalysts

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Nano Research 2024年第5期17卷 3872-3878页

作者： Yan Jiang Xuetong Yu Yuxia Ji Xunzhu Jiang Yalin Guo Tianbo Li Liang Gao Rui Lang Yanxiong Fang Botao Qiao Jinxiang Dong School of chemical Engineering and Light Industry Guangdong University of TechnologyGuangzhou 510006China Jieyang Branch of Chemistry and chemical Engineering guangdong laboratory(Rongjiang laboratory) Jieyang 515200China CAS key laboratory of Science and technology on Applied Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116024China guangdong provincial key laboratory of Plant Resources Biorefinery Guangzhou 510006China School of chemical Engineering and technology China University of Mining and TechnologyXuzhou 221116China

Alcohol-based disinfectants have protected people in the coronavirus disease 2019(COVID-19)pandemic,but olfactory stimuli of ethanol may evoke unpleasant memories associated with stressful situations in the devastating infectious *** smell of ethanol in household cleaning and disinfectant products can be covered up by the fragrance additives,and 3-hexenol is especially appreciated for the characteristic,strong odor of green *** production of 3-hexenol relies on the selective hydrogenation of 3-hexyn-1-ol,where Lindlar catalyst is normally used for the superior *** achieving such catalytic transformation in ethanol solution seems as a direct way to produce a disinfectant with green aroma,a popular consumer product in the post-COVID era,severe leaching of toxic Pb hinders Lindlar catalyst as a promising *** find that the Fe_(2)O_(3) supported Pd single-atom catalyst is highly selective to fulfill semi-hydrogenation of 3-hexyn-1-ol in 75%ethanol,and the aforementioned household product is readily generated after filtrating the stable,solid catalyst out of reaction ***-atom catalysts have been frequently utilized for fine-chemical synthesis,while in this work they make stunning debut in practical manufacture of daily used products.

关键词： single-atom catalysis hydrogenation fragrance household product coronavirus disease 2019(COVID-19)

Rh(Ⅱ)-catalyzed intermolecular carboamination of pyridines via double Csp^(2)-H bond activations

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Science China Chemistry 2024年第1期67卷 374-382页

作者： Zhongfeng Luo Jingxing Jiang Lifang Zou Xiaoyu Zhou Junshan Liu Zhuofeng Ke Fengjuan Chen Huanfeng Jiang Wei Zeng key laboratory of Functional Molecular Engineering of guangdong Province School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510641China School of Materials Science and Engineering PCFM LabSun Yat-sen UniversityGuangzhou 510275China guangdong provincial key laboratory of Chinese Medicine Pharmaceutics School of Traditional Chinese MedicineSouthern Medical UniversityGuangzhou 510515China

We disclose the development of the Rh-catalyzed amine-directed remote 5,6-carboamination protocol of pyridines via dual Csp^(2)-H functionalizations.A variety of readily available 2-aminopyridines and 1,2,3-triazoles are allowed for coupling cyclization to access polyfunctionalized *** studies including DFT calculations unveil that relay carbenoidelectrophilic addition to pyridines and the sequential pyridyl Csp^(2)-H amination are involved in this *** postsynthetic utility of this methodology is showcased by versatile and site-selective modification of azaindoles.

关键词： Rh-catalysis azaindoles pyridyl Csp^(2)-H bond carboamination coupling-cyclization

Chemoselective epoxidation of electron-deficient olefins with molecular oxygen via conjugated olefins epoxidation and BHT hydroxylation

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Science China Chemistry 2024年

作者： Jia Nie Huanfeng Jiang Chuanle Zhu School of Chemistry and chemical Engineering Key Lab of Functional Molecular Engineering of Guangdong ProvinceSouth China University of Technology guangdong provincial key laboratory of Technique and Equipment for Macromolecular Advanced Manufacturing South China University of Technology

The chemoselective epoxidation of electron-deficient olefins in the presence of electron-rich alkene moieties is *** chemoselective epoxidation strategy undergoes a conjugated olefin epoxidation and BHT hydroxylation process to give various useful oxiranes in high yields,especially for the 2-substituted ***,this protocol features mild conditions,is transition-metal free,operationally simple,and gram-scalable,and tolerates diverse functional *** candidate HSD-16 is synthesized smoothly by this *** studies indicate molecular oxygen is the terminal oxidant and the O-source of the oxiranes.

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A novel and promising engineering application of carbon dots:Enhancing the chloride binding performance of cement

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Chinese chemical Letters 2024年第6期35卷 409-416页

作者： Wu-Jian Long Yang Yu Chuang He guangdong provincial key laboratory of Durability for Marine Civil Engineering Key Lab of Coastal Urban Resilient InfrastructureMOECollege of Civil and Transportation EngineeringShenzhen UniversityShenzhen 518060China

Corrosion of reinforcement induced by chloride invasion is extensively considered as the dominating deterioration mechanism of reinforced concrete(RC)structures,leading to serious safety hazards and tremendous economic ***,it still lacks well dispersive and cost-efficient nanomaterials to improve the anti-chloride-corrosion ability of RC ***,specific carbon dots(CDs)with high dispersity and low cost are deliberately designed,successfully prepared by hydrothermal processing,and then firstly applied to immensely enhance chloride binding performance of cement,thereby contributing to suppressing the corrosion of ***,the tailored CDs are composed of the carbon core with highly crystalline sp^(2)C structures and oxygen-containing groups connecting on the carbon core;The typical equilibrium test confirms that with respect to that of the blank cement paste,the chloride binding capacity of cement paste involving 0.2 wt%(by weight of cement)CDs is increased by 109% after 14-day exposure to 3 mol/L Na Cl solution;according to comprehensive analyses of phase compositions,the chloride binding mechanism of CDs-modified cement is rationally attributed to the fact that the incorporation of CDs advances the formation of calcium silicate hydrate(C-S-H)gels and Friedel's salt(Fs),thus enormously enhancing the physically adsorbed and chemically bound chloride ions of cement *** work not only firstly provides a novel high-dispersity and low-cost nanomaterial toward the durability enhancement of RC structures,but also broadens the application of CDs in the field of engineering,conducing to stimulating their industrialization development.

关键词： Carbon dots Chloride binding Cement Chloride binding mechanism Friedel’s salt

Enhancing green Ammonia Electrosynthesis Through Tuning Sn Vacancies in Sn‑Based MXene/ MAX Hybrids

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Nano-Micro Letters 2024年第5期16卷 154-168页

作者： Xinyu Dai Zhen‑Yi Du Ying Sun Ping Chen Xiaoguang Duan Junjun Zhang Hui Li Yang Fu Baohua Jia Lei Zhang Wenhui Fang Jieshan Qiu Tianyi Ma key laboratory for green Synthesis and Preparative Chemistry of Advanced Materials of Liaoning Province College of ChemistryInstitute of Clean Energy ChemistryLiaoning UniversityShenyang 110036People’s Republic of China State key laboratory of Clean and Efficient Coal Utilization Taiyuan University of TechnologyTaiyuan 030024People’s Republic of China School of Chemistry and chemical Engineering Anhui UniversityHefei 230601People’s Republic of China School of chemical Engineering The University of AdelaideAdelaideSA 5005Australia State key laboratory of High‑Efficiency Utilization of Coal and green chemical Engineering College of Chemistry and Chemical EngineeringNingxia UniversityYinchuan 750021NingxiaPeople’s Republic of China School of Science RMIT UniversityMelbourneVIC 3000Australia guangdong provincial key laboratory of Advanced Energy Storage Materials School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510640People’s Republic of China College of chemical Engineering State Key Laboratory of Chemical Resource EngineeringBeijing University of Chemical TechnologyBeijing 100029People’s Republic of China

Renewable energy driven N_(2) electroreduction with air as nitrogen source holds great promise for realizing scalable green ammonia ***,relevant out-lab research is still in its ***,a novel Sn-based MXene/MAX hybrid with abundant Sn vacancies,Sn@Ti_(2)CTX/Ti_(2)SnC–V,was synthesized by controlled etching Sn@Ti_(2)SnC MAX phase and demonstrated as an efficient electrocatalyst for electrocatalytic N2 *** to the synergistic effect of MXene/MAX heterostructure,the existence of Sn vacancies and the highly dispersed Sn active sites,the obtained Sn@Ti2CTX/Ti_(2)SnC–V exhibits an optimal NH_(3) yield of 28.4μg h^(−1) mg_(cat)^(−1) with an excellent FE of 15.57% at−0.4 V versus reversible hydrogen electrode in 0.1 M Na_(2)SO_(4),as well as an ultra-long ***,this catalyst represents a satisfactory NH3 yield rate of 10.53μg h^(−1) mg^(−1) in the home-made simulation device,where commercial electrochemical photovoltaic cell was employed as power source,air and ultrapure water as feed *** as-proposed strategy represents great potential toward ammonia production in terms of financial cost according to the systematic technical economic *** work is of significance for large-scale green ammonia production.

关键词： green ammonia synthesis N2 electroreduction Renewable energy Sn MXene/MAX hybrid