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Carbon energy 2024年第1期6卷 255-266页

作者： Qianying Lin Jiwu Zhao Pu Zhang Shuo Wang Ying Wang Zizhong Zhang Na Wen Zhengxin Ding Rusheng Yuan Xuxu Wang Jinlin Long state key laboratory of photocatalysis on energy and environment College of ChemistryFuzhou UniversityFuzhouChina

Efficient photocatalytic reduction of CO_(2) to high-calorific-value CH4,an ideal target product,is a blueprint for C_(1)industry relevance and carbon neutrality,but it also faces great ***,we demonstrate unprecedented hybrid SiC photocatalysts modified by Fe-based cocatalyst,which are prepared via a facile impregnation-reduction method,featuring an optimized local electronic *** exhibits a superior photocatalytic carbon-based products yield of 30.0μmol g^(−1) h^(−1) and achieves a record CH_(4) selectivity of up to 94.3%,which highlights the effectiveness of electron-rich Fe cocatalyst for boosting photocatalytic performance and ***,the synergistic effects of directional migration of photogenerated electrons and strongπ-back bonding on low-valence Fe effectively strengthen the adsorption and activation of reactants and intermediates in the CO_(2)→CH_(4) *** study inspires an effective strategy for enhancing the multielectron reduction capacity of semiconductor photocatalysts with low-cost Fe instead of noble metals as cocatalysts.

关键词： artificial synthesis of CH_(4) electronic structure optimization Fe species cocatalyst photocatalytic CO_(2) reduction SiC

S-scheme heterojunction of crystalline carbon nitride nanosheets and ultrafine WO_(3)nanoparticles for photocatalytic CO_(2)reduction

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Journal of environmental Sciences 2024年第6期140卷 103-112页

作者： Gongjie Chen Ziruo Zhou Bifang Li Xiahui Lin Can Yang Yuanxing Fang Wei Lin Yidong Hou Guigang Zhang Sibo Wang state key laboratory of photocatalysis on energy and environment College of ChemistryFuzhou UniversityFujian 350116China

Highly crystalline carbon nitride polymers have shown great opportunities in overall water photosplitting;however,their mission in light-driven CO_(2)conversion remains to be *** this work,crystalline carbon nitride(CCN)nanosheets of poly triazine imide(PTI)embedded with melon domains are fabricated by KCl/LiCl-mediated polycondensation of dicyandiamide,the surface of which is subsequently deposited with ultrafine WO_(3)nanoparticles to construct the CCN/WO_(3)heterostructure with a S-scheme *** characterizations have been conducted to reveal the compositions and structures of the S-scheme CCN/WO_(3)hybrid,featuring strengthened optical capture,enhanced CO_(2)adsorption and activation,attractive textural properties,as well as spatial separation and directed movement of light-triggered charge *** mild conditions,the CCN/WO_(3)catalyst with optimized composition displays a high photocatalytic activity for reducing CO_(2)to CO in a rate of 23.0μmol/hr(i.e.,2300μmol/(hr·g)),which is about 7-fold that of pristine CCN,along with a high CO selectivity of 90.6%against ***,it also manifests high stability and fine reusability for the CO_(2)conversion *** CO_(2)adsorption and conversion processes on the catalyst are monitored by in-situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS),identifying the crucial intermediates of CO_(2)^(*)-,COOH^(*)and CO^(*),which integrated with the results of performance evaluation proposes the possible CO_(2)reduction mechanism.

关键词： Crystalline carbon nitride photocatalysis CO_(2)reduction S-scheme WO_(3)

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

Nitrogen-doped titanium dioxide/schwertmannite nanocomposites as heterogeneous photo-Fenton catalysts with enhanced efficiency for the degradation of bisphenol A

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Journal of environmental Sciences 2024年第9期143卷 1-11页

作者： Xing-Xing Qiao Yu-Hang Xu Xiang-Ji Liu Sai-Le Chen Zhou Zhong Ya-Feng Li Jian Lü Fujian Provincial key laboratory of Soil environmental Health and Regulation College of Resources and EnvironmentFujian Agriculture and Forestry UniversityFuzhou 350002China state key laboratory of photocatalysis on energy and environment Fuzhou UniversityFuzhou 350116China

Potential health risks related to environmental endocrine disruptors(EEDs)have aroused research hotspots at the forefront of water treatment ***,nitrogen-doped titanium dioxide/schwertmannite nanocomposites(N-TiO_(2)/SCH)have been successfully developed as heterogeneous catalysts for the degradation of typical EEDs via photo-Fenton *** to the sustainable Fe(Ⅲ)/Fe(Ⅱ)conversion induced by photoelectrons,as-prepared N-TiO_(2)/SCH nanocomposites exhibit much enhanced efficiency for the degradation of bisphenol A(BPA;ca.100% within 60 min under visible irradiation)in a wide pH range of 3.0-7.8,which is significantly higher than that of the pristine schwertmannite(ca.74.5%)or N-TiO_(2)(ca.10.8%).In this photo-Fenton system,the efficient degradation of BPA is mainly attributed to the oxidation by hydroxyl radical(·OH)and singlet oxygen(^(1)O_(2)).Moreover,the possible catalytic mechanisms and reaction pathway of BPA degradation are systematically investigated based on analytical and photoelectrochemical *** work not only provides a feasible means for the development of novel heterogeneous photo-Fenton catalysts,but also lays a theoretical foundation for the potential application of mineral-based materials in wastewater treatment.

关键词： Titanium dioxide Schwertmannite Fenton reaction environmental endocrine disruptors photocatalysis

Iron–doped bismuth oxybromides as visible-light-responsive Fenton catalysts for the degradation of atrazine in aqueous phases

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Journal of environmental Sciences 2024年第3期137卷 321-332页

作者： Yong-Li Cai Yu-Hang Xu Ji-Zun Xiang Zhi-Qiang Zhang Qiu-Xiang He Ya-Feng Li Jian Lü Fujian Provincial key laboratory of Soil environmental Health and Regulation College of Resources and EnvironmentFujian Agriculture and Forestry UniversityFuzhou 350002China state key laboratory of photocatalysis on energy and environment Fuzhou UniversityFuzhou 350116China

Pesticides and its degradation products,being well–known residues in soil,have recently been detected in many water bodies as pollutants of emerging concerns,and thus there is a contemporary demand to develop viable and cost–effective techniques for the removal of related organic pollutants in aqueous ***,a visible-light-responsive Fenton system was constructed with iron–doped bismuth oxybromides(Fe–BiOBr)as the *** the advantage of sustainable Fe(Ⅲ)/Fe(Ⅱ)conversion and optimized H_(2)O_(2)utilization,the optimal Fe–BiOBr–2 catalyst showed an excellent atrazine removal efficiency of 97.61%in 120 min,which is superior than the traditional homogeneous Fenton and the majority of heterogeneous processes documented in the *** this photo–Fenton system,hydroxyl(·OH)and superoxide(·O_(2)^(-))radicals were dominant active species contributed to the oxidative degradation of *** to the production of various active radicals,five degradation pathways were proposed based on the identification of intermediates and degradation ***,this work not only demonstrates a fundamental insight into creating highly efficient and atom economic photo-Fenton systems,but also provides a complementary strategy for the treatment of organic pollutants in water.

关键词： Bismuth oxybromide Photo–Fenton Atrazine Catalytic degradation

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

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Enhancing CO2 cycloaddition through ligand functionalization:A case study of UiO-66 metal-organic frameworks

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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Intermolecular reductive coupling of aliphatic ketones with alkynes and alkenes by BCN photocatalysts

结构化学 2024年第2期43卷 9-12页

作者： Ruowen Liang Chao Zhang Guiyang Yan Fujian Province key laboratory of Featured Biochemical and Chemical Materials Ningde Normal UniversityNingde352100PR China state key laboratory of photocatalysis on energy and environment Fuzhou University Fuzhou350002PR China state key laboratory of photocatalysis on energy and environment Fuzhou University Fuzhou350002PR China

The synthesis of cyclic carbonates from CO2 and epoxides offers a remarkable 100％atomic *** literature describes the CO2 cycloaddition mechanism predominantly as an"epoxide activation"pathway[1].This process can be effectively facilitated by heterogeneous catalysts possessing Lewis acidity,potentially optimising the capture and activation of the epoxide via metal-oxygen ***-organic frameworks(MOFs)have recently garnered attention as new catalysts,credited to their structural adaptability and multifunctional ***,MOFs with exposed metal sites function as Lewis acid sites,thus enhancing the cycloaddition *** numerous researchers emphasize the pivotal role of epoxide activation in the CO2 cycloaddition process,the challenge of activating inherently stable CO2 molecules often remains *** CO2 activation can potentially reduce the energy barriers of the reaction,thereby enhancing the overall *** prior studies on MOFs'catalytic activities for CO2 cycloaddition primarily emphasise their Lewis acidity sites[2,3],with scant attention to the syn-ergistic effects between the Lewis acid and base sites.

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Science China Chemistry 2024年

作者： Yanping Xia Luyang Sun Jiajia Cheng Sibo Wang Meifang Zheng Xinchen Wang state key laboratory of photocatalysis on energy and environment College of ChemistryFuzhou University

A photocatalytic process was developed for intermolecular reductive coupling of aliphatic ketones with alkynes/alkenes to furnish tertiary *** studies support that boron carbonitrides (BCN) promote the single electron reduction of unactivated aliphatic ketones to generate ketyl radicals with visible light irradiation,which then react with alkynes and alkenes to afford the allylic and aliphatic alcohols,*** heterogeneous photocatalytic system is compatible with diverse substrates including pharmaceutical-related molecules (43 examples) with reusability and scale-up experiments,verifying the complementary synthetic utility of this method to the homogeneous catalysts.

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Extended light absorption and accelerated charge migration in ultrathin twisted carbon nitride nanoplates for efficient solar hydrogen production

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Science China Chemistry 2024年第7期67卷 2215-2223页

作者： Yanmin Zou Shiyao Li Dandan Zheng Jianyong Feng Sibo Wang Yidong Hou Guigang Zhang state key laboratory of photocatalysis on energy and environment College of ChemistryFuzhou UniversityFuzhou 350108China College of environment and Safety Engineering Fuzhou UniversityFuzhou 350108China Collaborative Innovation Center of Advanced Microstructures National Laboratory of Solid State MicrostructuresCollege of Engineering and Applied SciencesNanjing UniversityNanjing 210093China

Polymeric carbon nitride has been widely developed as a promising photocatalyst for solar hydrogen production via photocatalytic water ***,pristine carbon nitride prepared by traditional solid-state polymerization usually encounters issues such as rapid carrier recombination and insufficient absorption of visible light below 460 ***,poly(heptazine imide)with a distinctive nanoplate structure was synthesized in a binary molten salt of NaCl–CaCl_(2).The salt template allows the formation of the thin nanoplate structure,which promotes the charge separation and ***,the intercalation of Ca^(2+)ions between the conjugated layers endows the activation of n–π*electron transition due to the distortion of in-plane heptazine ***,the optimized poly(heptazine imide)nanoplates achieve an apparent quantum efficiency of up to 17.3%at 500 nm for photocatalytic hydrogen production from *** work shares new idea for rational control of the optical absorption and charge carrier dynamics of poly(heptazine imide).

关键词： photocatalysis poly heptazine imide nanoplates ion intercalation hydrogen production

Photocatalytic oxidation of methane to methanol over zinc titanate supported silver catalysts

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Journal of Rare Earths 2024年第5期42卷 899-906,I0004页

作者： Yuyan Gan Jinbi Huang Qian Lv Yanru Li Lizhi Wu YU Tang Yuanxing Fang Pengfei Zhu Li Tan Institute of Molecule Catalysis and In-Situ/Operando Studies State Key Laboratory of Photocatalysis on Energy and EnvironmentCollege of ChemistryFuzhou UniversityFuzhou350108China School of environmental Science and Engineering Shaanxi University of Science and TechnologyXi'an 70021China

The direct activation of methane under mild condition to achieve highly selective of oxygenates is a challenging *** this study,a well dispersed silver supported ZnTiO_(3) catalyst was prepared to achieve selective preparation of methanol from methane and water under mild condition.X-ray diffraction,transmission electron microscopy and X-ray photoelectron spectroscopy characterizations demonstrate that silver species are uniformly dispersed on ZnTiO_(3) surface in the form of metallic silver *** photoelectric characterizations reveal that the addition of silver species enhances light absorption and promotes charge separation of the *** the reaction conditions of 50℃and 3 MPa,the methanol is obtained as the only liquid product over the designed Ag/ZnTiO_(3) catalyst under light *** this photocatalytic process,the holes generated by ZnTiO_(3) activate water to produce intermediate·OH,which further reacts with methane to synthesize *** silver species as co-catalysts extend the light absorption range of ZnTiO_(3) as well as promote charge separation.

关键词： Photocatalytic Methane oxidation Zinc titanate Silver Methanol