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Dynamic cooperations between lattice oxygen and oxygen vacancies for photocatalytic ethane dehydrogenation by a self-restoring LaVO_(4)catalyst

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Chinese Chemical Letters 2024年第3期35卷 171-176页

作者： Fen Wei Weichao Xue Zhiyang Yu Xue Feng Lu Sibo Wang Wei Lin Xinchen Wang State Key Laboratory of Photocatalysis on Energy and environment College of ChemistryFuzhou UniversityFuzhou 350108China

Thermocatalytic nonoxidative ethane dehydrogenation(EDH)is a promising strategy for ethene production but suffers from intense energy consumption and poor catalyst durability;exploring technology that permits efficient EDH by solar energy remains a giant ***,we present that an oxygen vacancy(O_v)-rich LaVO_(4)(LaVO_(4)-O_v)catalyst is highly active and stable for photocatalytic EDH,through a dynamic lattice oxygen(O_(latt.))and O_(v)co-mediated *** by simulated sunlight at mild conditions,LaVO_(4)-O_(v)effectively dehydrogenates undiluted ethane to produce C_(2)H_(4)and CO with a conversion of 2.3%.By loading a small amount of Pt cocatalyst,the evolution and selectivity of C_(2)H_(4)are enhanced to 275μmol h^(-1)g^(-1)and 96.8%.Of note,LaVO_(4)-O_(v)appears nearly no carbon deposition after the *** isotope tracked reactions reveal that the consumed O_(latt.)recuperates by exposing the used catalyst with O_(2),thus establishing a dynamic cycle of O_(latt.)and achieving a facile catalyst regeneration to preserve its intrinsic *** refreshed LaVO_(4)-O_(v)exhibits superior reusability and delivers a turnover number of about *** O_(v)promotes photo absorption,boosts ethane adsorption/activation,and accelerates charge separation/transfer,thus improving the photocatalytic *** possible photocatalytic EDH mechanism is proposed,considering the key intermediates predicted by density functional theory(DFT)and monitored by in-situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS).

关键词： Photocatalysis Ethane dehydrogenation Ethene LaVO_(4) Oxygen vacancy

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Pathways toward a pollution-free planet and challenges

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Frontiers of environmental science & Engineering 2024年第6期18卷 3-8页

作者： Jiuhui Qu Jiaping Chen School of environment Tsinghua UniversityBeijing 100084China college of chemistry and environmental Engineering Shenzhen UniversityShenzhen 518060China

The mission of“Establishment of Zero-Pollution Earth”defined by United Nations environment Programme aims at creation of a clean,safe and prosperous home for all human *** is of rational choice from each individual to protect our environment and demonstrates our great ambition to achieve our *** key message given in this article is that,zero pollution does not mean no discharge of pollutants and instead it can be achievable through optimizing and controlling a sound balance between pollutants discharge and capacities of decontamination through treatment and natural environmental accumulation,which can be termed as“Principle of Equilibrium”between pollution and *** on this principle,we propose and illustrate several key factors and synergistic pathways toward a pollution-free planet:quantitative determination on purification and wastewater;source control through green measures;minimization of negative side-effects;precise management through digitalized systems;and keeping sound balance between pollutants and natural *** should be noted that we would face a series of difficulties and challenges in moving forward to“Zero-Pollution Earth”.We should further develop theories,principles and tools to achieve the balance between quantity of pollutants and decontamination *** should work together to break through the bottleneck limited by“Principle of equilibrium”to establish new environmental remediation systems leading to“Zero-Pollution Earth”.

关键词： Wastewater treatment Resources Recovery Greenhouse gases Energy Pollution-free

High efficiency removal of NO using waste calcium carbide slag by facile KOH modification

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Journal of environmental sciences 2024年第5期139卷 182-192页

作者： Fang Wang Hui Li Jiyun Gao Na Geng Enzhu Jiang Futing Xia Mingwu Xiang Lijuan Jia Ping Ning School of chemistry and environment Yunnan Minzu UniversityKunming 650504China Faculty of environmental science and Engineering Kunming University of Science and TechnologyKunming 650500China

Waste calcium carbide slags(CS),which are widely applied to desulfurisation,are not typically used in ***,to well achieve waste control by waste,a facile and highefficiency denitration strategy is developed using KOH to modify the calcium carbide slags(KCS).Various KCS samples were investigated using a series of physical and chemical *** performance test results showed that the KOH concentration and reaction temperature are the main factors affecting the denitration efficiency of KCS,and CS modified with 1.5 mol/L KOH(KCS-1.5)can achieve 100% denitration efficiency at 300℃.Such excellent removal efficiency is due to the catalytic oxidation of the oxygen-containing functional groups derived from the *** studies showed that KOH treatment significantly increased the concentration of oxygen vacancies,nitro compounds,and basic sites of *** study provides a novel strategy for the resource utilisation of waste CS in the future.

关键词： Waste Carbide slag KOH Effective denitration

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Acidic electroreduction CO_(2)to formic acid via interfacial modification of Bi nanoparticles at industrial-level current

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Nano Research 2024年第7期17卷 5817-5825页

作者： Tian Dong Hongdong Li Zhenhui Wang Yanling Geng Rui Chang Xiaofeng Tian Jianping Lai Shouhua Feng Lei Wang Key Laboratory of Eco-Chemical Engineering International Science and Technology Cooperation Base of Eco-Chemical Engineering and Green ManufacturingCollege of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042China Shandong Engineering Research Center for Marine environment Corrosion and Safety Protection College of Environment and Safety EngineeringQingdao University of Science and TechnologyQingdao 266042China

Electrocatalytic CO_(2)reduction reaction(CO_(2)RR)in acidic media is a promising approach to overcome the unavoidable formation of carbonates in alkaline or neutral ***,the proton-rich environment near the catalyst surface favors hydrogen evolution reactions(HER),leading to lower energy efficiency of the desired products,especially in industrial-level current ***,quaternary ammonium cationic surfactant(cetyltrimethylammonium bromide(CTAB))was introduced into acidic electrolyte to modulate the interfacial microenvironment,which greatly enhanced CO_(2)electroreduction to formic acid(HCOOH)at the Bi/C nanoparticles *** a Bi/C nanoparticles electrode with CTAB added,constant production of formic acid was enabled with a cathodic energy efficiency of>40%and maximum FE_(HCOOH)(FE=Faradaic efficiency)of 86.2%at−400 mA·cm^(−2)over 24 *** with in-situ attenuated total reflection Fourier transform infrared spectroscopy,the concentration of*OCHO intermediates significantly increased after CTAB modification,confirming that the hydrophobic interface microenvironment formed by dynamic adsorption of positively charged long alkyl chains on Bi/C nanoparticle electrodes inhibited HER and improved the selectivity of CO_(2)RR to HCOOH.

关键词： acidic media CO_(2)electrolysis electrolyte additive hydrophobic interfacial microenvironment industrial-level current

Defect and nanostructure engineering of polymeric carbon nitride for visible-light-driven CO2 reduction

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MoO_(x) nanoclusters on Mo-doped TiO_(2) nanosheets with enhanced singlet oxygen generation and sulfide conversion abilities for photocatalytic aerobic oxidative desulfurization

结构化学 2024年第3期43卷 10-18页

作者： Ziruo Zhou Wenyu Guo Tingyu Yang Dandan Zheng Yuanxing Fang Xiahui Lin Yidong Hou Guigang Zhang Sibo Wang State Key Laboratory of Photocatalysis on Energy and environment College of ChemistryFuzhou UniversityFuzhou350116China college of environment and Safety Engineering Fuzhou UniversityFuzhou350108China

Sunlight-induced photocatalytic carbon dioxide(CO2)reduction to energy-rich chemicals by metal-free polymeric carbon nitride(CN)semiconductor is a promising tactic for sustained solar fuel ***,the reaction efficiency of CO2 photoreduction is restrained seriously by the rapid recombination of photogenerated carriers on CN ***,we incorporate 2-aminopyridine molecule with strong electron-withdrawing group into the skeleton edge of CN layers through a facile one-pot thermal polymerization strategy using urea as the precursor,which renders a modified carbon nitride(ACN)with extended optical harvesting,abundant nitrogen defects and ultrathin nanosheet ***,the ACN photocatalyst with desirable structural features attains enhanced separation and migration of photoexcited charge *** visible light irradiation with Co(bpy)32+as a cocatalyst,the optimized ACN sample manifests a high CO2 deoxygnative reduction activity and high sta-bility,providing a CO yielding rate of 17 μmol h-1,which is significantly higher than that of pristine *** key intermediates engaged in CO2 photoreduction reaction are determined by the in situ diffuse reflectance infrared Fourier transform spectroscopy,which sponsors the construction of the possible photocatalytic CO2 reduction mechanism on ACN nanosheets.

关键词： Carbon nitride Photocatalysis CO_2 reduction Nitrogen defects Nanosheets

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science China chemistry 2024年第1期67卷 408-414页

作者： Suting Xie Xinyu Zhao Dongxiao Wang Huawei Yang Lixia Yang Liangjiu Bai Donglei Wei Wenxiang Wang Ying Liang Hou Chen Shaojun Guo college of chemistry and Materials science Ludong UniversityYantai 264025China college of Materials science and Engineering Peking UniversityBeijing 100871China

Photocatalytic aerobic oxidation desulfurization(PAODS)is a promising and sustainable alternative to conventional,energyintensive desulfurization techniques for petroleum ***,its development is greatly plagued by the low capability in generating highly reactive oxygen species and sluggish kinetics of sulfide oxidation of reported *** we report a class of MoO_(x)nanocluster decorated on ultrathin Mo-doped TiO_(2)nanosheet(MoO_(x)/MoTiO)catalyst for efficiently facilitating the photocatalytic aerobic oxidation of *** demonstrate that MoO_(x)/MoTiO can not only promote the generation of highly reactive singlet oxygen(^(1)O_(2))but also enhance the aerobic conversion of sulfides,which leads to a record dibenzothiophene oxidation activity of 3.90 mmol g^(-1)h^(-1).The multiple experimental characterizations and density functional theory calculations collectively reveal that the doped-Mo sites can interact with the photogenerated excitons,enabling directly energy transfer generation of^(1)O_(2)through a new exciton modulation mechanism,and the coordination unsaturated MoO_(x)clusters play the role of co-catalyst to enhance the separation of charge carriers,and effectively catalyze the reaction between sulfides and1O_(2)to form sulfones.

关键词： titanium dioxide photocatalytic aerobic oxidation desulfurization dibenzothiophene singlet oxygen

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Fabrication of Silane and Desulfurization Ash Composite Modified Polyurethane and Its Interfacial Binding Mechanism

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Journal of Wuhan University of Technology(Materials science) 2024年第2期39卷 288-297页

作者：吴旺华 CHEN Shuichang YE Haodong 李世迁 LIN Yuanzhi 陈庆华 XIAO Liren college of chemistry and Materials science Fujian Normal UniversityFuzhou 350117China college of Materials and Package Engineering Fujian Provincial Key Lab of Coastal Basin EnvironmentFujian Polytechnic Normal UniversityFuqing 350300China college of Agriculture Guangxi UniversityGuangxi 530004China

Polyurethane/desulfurization ash(PU/DA)composites were synthesized using"one-pot method",with the incorporation of a silane coupling agent(KH550)as a"molecular bridge"to facilitate the integration of DA as hard segments into the PU molecular *** effects of DA content(φ)on the mechanical properties,thermal stability,and hydrophobicity of PU,both before and after the addition of KH550,were thoroughly *** results of microscopic mechanism analysis confirmed that KH550 chemically modified the surface of DA,facilitating its incorporation into the polyurethane molecular chain,thereby significantly enhancing the compatibility and dispersion of DA within the PU *** the mass fraction of modified DA(MDA)reached 12%,the mechanical properties,thermal stability,and hydrophobicity of the composites were substantially improved,with the tensile strength reaching 14.9 MPa,and the contact angle measuring 100.6°.

关键词： polyurethane silane coupling agent desulfurization ash modification mechanical property hydrophobicity thermal stability

Regulate electric double layer for one-step synthesize and modulate the morphology of(oxy)hydroxides

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Nano Research 2024年第5期17卷 3675-3683页

作者： Jiaxin Liu Yue Shi Yanli Gu Zheng Lv Liang Zhao Yu Yang Tianrong Zhan Jianping Lai Lei Wang State Key Laboratory Base of Eco-Chemical Engineering International Science and Technology Cooperation Base of Eco-chemical Engineering and Green ManufacturingCollege of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042China Shandong Engineering Research Center for Marine environment Corrosion and Safety Protection College of Environment and Safety EngineeringQingdao University of Science and TechnologyQingdao 266042China

FeOOH have received considerable attention due to their natural abundance and *** the significant progress achieved,the one-step synthesis of integrated FeOOH is still a major ***,the current research on FeOOH catalyst still suffers from the unclear mechanism of controlling ***,density functional theory(DFT)calculations and X-ray photoelectron spectroscopy(XPS)demonstrated the strong electron-capturing and hydrogen absorption ability of Co in FeOOH,which further promotes the formation and stabilization of *** used a one-step electrodeposition method to synthesize Co introduced FeOOH integrated electrocatalyst and propose to introduce ions with different valence states to regulate the morphology of FeOOH by precise modulation of electric double layer(EDL)composition and *** prepared Co-FeOOH-K^(+)has a larger electrochemically active surface area(ECSA)(325 cm^(2))and turnover frequency(TOF)value(0.75 s^(-1)).In the electrochemical experiments of an alkaline anion exchange membrane electrolyzer,Co-FeOOH-K^(+)shows better oxygen evolution performance than commercial RuO_(2) under industrial production conditions and has good industrial application prospects.

关键词： integrated(oxy)hydroxides electrodeposition electric double layer(EDL) oxygen evolution reaction(OER) morphology regulation

Highly active organocatalyst from a trivalent phosphazenium salt for ring-opening copolymerization of epoxides and cyclic anhydrides enhanced by hydrogen bonding interactions

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science China chemistry 2024年第9期67卷 3111-3120页

作者： Chunhuan Jiang Junqi Wang Xiaoyu Liu Xiaoxia You Ronglin Zhong Chuanli Ren Zhibo Li Key Laboratory of Biobased Polymer Materials Shandong Provincial Education Department College of Polymer Science and EngineeringQingdao University of Science and Technology Laboratory of Theoretical and Computational chemistry Institute of Theoretical Chemistry College of Chemistry Jilin University college of Chemical Engineering Qingdao University of Science and Technology

It is highly desirable to develop simple organocatalysts for the controlled ring-opening alternating copolymerization（ROAC） of epoxides and cyclic anhydrides, leading to high molecular weight polyesters. Hence, a phosphazenium salt, namely tri[tris（dimethylamino）phosphoranylidenamino]phosphonium chloride（P4+Cl-）, is developed as a catalyst for the ROAC of epoxides and cyclic anhydrides. Surprisingly, the combination of P4+Cl-with a protonic initiator, such as 1,4-benzenedimethanol（BDM）exhibited high efficiency in the copolymerization of propylene oxide（PO） and phthalic anhydride（PA）. This led to the production of polyester with an exceptional high molecular weight（M_n） of up to 126 k Da, which represented a rare example of poly（PO-alt-PA） with Mnsurpassing 100 k Da. Note that the core P atom is trivalent status and the tris[tris（dimethylamino）]phosphoranyl group will share one proton in the P4+Cl-salt. Once combined with protonic species, the P4+Cl-will not only serve as a proton acceptor but also as a hydrogen bonding donor for the cyclic anhydrides. Therefore, it was assumed that the P4+plus proton served dual role in mimic of base/urea pair to effectively catalyze ROAC, which was supported by density functional theory（DFT） calculations.

关键词： ring-opening copolymerization organocatalyst epoxides cyclic anhydrides phosphazenium salt

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