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Highly selective photocatalytic reduction of CO_(2) to CH_(4) on electron-rich Fe species cocatalyst under visible light irradiation

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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

Two-Dimensional Perovskite Single Crystals for High-Performance X-ray Imaging and Exploring MeV X-ray Detection

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Energy & Environmental Materials 2024年第1期7卷 139-146页

作者： Xieming Xu Yiheng Wu Yi Zhang Xiaohui Li Fang wang Xiaoming Jiang Shaofan Wu Shuaihua wang Key Laboratory of Optoelectronic Materials Chemistry and Physics Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China University of Chinese Academy of Sciences Beijing 100049China Division of Nuclear Technology and Applications Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049China Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108China

Scintillation semiconductors play increasingly important medical diagnosis and industrial inspection ***,two-dimensional(2D)perovskites have been shown to be promising materials for medical X-ray imaging,but they are mostly used in low-energy(≤130 keV)*** detection of MeV X-rays,which ensure thorough penetration of the thick shell walls of containers,trucks,and aircraft,is also highly desired in practical industrial ***,scintillation semiconductors for high-energy X-ray detection are currently ***,This paper reports a 2D(C_(4)H_(9)NH_(3))_(2)PbBr_(4)single crystal with outstanding sensitivity and stability toward X-ray radiation that provides an ultra-wide detectable X-ray range of between 8.20 nGy_(air)s^(-1)(50 keV)and 15.24 mGy_(air)s^(-1)(9 MeV).The(C_(4)H_(9)NH_(3))_(2)PbBr_(4)single-crystal detector with a vertical structure is used for high-performance X-ray imaging,delivering a good spatial resolution of 4.3 Ip mm^(-1)in a plane-scan imaging *** ionic migration in the 2D perovskite enables the vertical device to be operated with hundreds of keV to MeV X-ray radiation at high bias voltages,leading to a sensitivity of 46.90μC Gy_(air)-1 cm^(-2)(-1.16 Vμm^(-1))with 9 MeV X-ray radiation,demonstrating that 2D perovskites have enormous potential for high-energy industrial applications.

关键词： MeV X-ray detection single-crystal X-ray detectors two-dimensional perovskites X-ray imaging

Synergistic effects of peroxydisulfate on UV/O3 process for tetracycline degradation:Mechanism and pathways

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Chinese Chemical Letters 2024年第10期35卷 434-439页

作者： Fengrui Yang Debing wang Xinying Zhang Jie Zhang Zhichao Wu Qiaoying wang State Key Laboratory of Pollution Control and Resource Reuse Shanghai Institute of Pollution Control and Ecological Security School of Environmental Science and Engineering Tongji University Fujian Provincial Engineering Research Center of Rural Waste Recycling Technology College of Environment & Safety Engineering Fuzhou University

Tetracycline（TC） as a typical emerging pollutant is becoming a serious threat to the environment and human health. A combined advanced oxidation technology of UV/Ozone（O3）/peroxydisulfate（PDS） process was developed to explore an efficient and economic treatment process of TC in wastewater. Furthermore,the reactive sites and transformation pathways of TC were explored and the toxicity of the intermediates was quantified with a quantitative structure-activity relationship（QSAR） assessment. The degradation performance of TC was substantially enhanced in UV/O3/PDS process with a kobsof 0.0949 min-1,which was 2.3 times higher than UV/O3and 3.2 times than sole UV. The results demonstrated that there was a superior synergistic effect of PDS on UV/O3processes for the degradation of TC. Electron paramagnetic resonance（EPR） analysis and quenching experiments show that·OH, SO4·-, O2·-and1O2all contributed to TC degradation in the UV/O3/PDS process and exhibited a synergistic effect, which inhibited the generation of harmful products. In addition, the UV/O3/PDS system can effectively degrade TC in a wide range of substrate concentrations and pH, and also showed excellent adaptability to various concentrations of anions（Cl-and HCO3-）. This study proves the feasibility of UV/O3/PDS process for treating TC contaminated wastewater with complicated water matrix.

关键词： Degradation Synergistic effect Tetracycline UV/ozonation/peroxydisulfate Wastewater

Conditional selection with CNN augmented transformer for multimodal affective analysis

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CAAI Transactions on Intelligence Technology 2024年第4期9卷 917-931页

作者： Jianwen wang Shiping wang Shunxin Xiao Renjie Lin Mianxiong Dong Wenzhong Guo College of Computer and Data Science Fuzhou UniversityFuzhouChina College of Computer and Cyber Security Fujian Normal UniversityFuzhouChina Key Laboratory of Network Computing and Intelligent Information Processing Fuzhou UniversityFuzhouChina Digital Fujian Institute of Big Data Security Technology Fujian Normal UniversityFuzhouChina Department of Sciences and Informatics Muroran Institute of TechnologyMuroranJapan

Attention mechanism has been a successful method for multimodal affective analysis in recent years. Despite the advances, several significant challenges remain in fusing language and its nonverbal context information. One is to generate sparse attention coefficients associated with acoustic and visual modalities, which helps locate critical emotional se-mantics. The other is fusing complementary cross‐modal representation to construct optimal salient feature combinations of multiple modalities. A Conditional Transformer Fusion Network is proposed to handle these problems. Firstly, the authors equip the transformer module with CNN layers to enhance the detection of subtle signal patterns in nonverbal sequences. Secondly, sentiment words are utilised as context conditions to guide the computation of cross‐modal attention. As a result, the located nonverbal fea-tures are not only salient but also complementary to sentiment words directly. Experi-mental results show that the authors’ method achieves state‐of‐the‐art performance on several multimodal affective analysis datasets.

关键词： affective computing data fusion information fusion multimodal approaches

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

Facile synthesis of hierarchical NaX zeolite from natural kaolinite for efficient Knoevenagel condensation

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Chinese Journal of Chemical Engineering 2024年第1期65卷 75-84页

作者： Wen Xiao Peng Dong Chan wang Jingdong Xu Tiesen Li Haibo Zhu Tinghai wang Renwei Xu Yuanyuan Yue National Engineering Research Center of Chemical Fertilizer Catalyst College of Chemical EngineeringFuzhou UniversityFuzhou 350108China Qingyuan Innovation Laboratory Quanzhou 362801China Sinochem Quanzhou Energy Technology Co. Ltd.Quanzhou 362000China

Zeolite catalysts have found extensive applications in the synthesis of various fine ***,the micropores of zeolites impose diffusion limitations on bulky molecules,greatly reducing the catalytic ***,we explore an economic and environmentally friendly method for synthesizing hierarchical NaX zeolite that exhibits improved catalytic performance in the Knoevenagel condensation reaction for producing the useful fine chemical *** synthesis was achieved via a low-temperature activation of kaolinite and subsequent in-situ transformation strategy without any template or *** characterizations reveal that the synthesized NaX zeolite has both intercrystalline and intra-crystalline mesopores,smaller crystal size,and larger external specific surface area compared to commercial NaX *** mechanism investigations show that the inter-crystalline mesopores are generated by stacking smaller crystals formed from in-situ crystallization of the depolymerized kaolinite,and the intra-crystalline mesopores are inherited from the pores in the depolymerized *** synthesis strategy provides an energy-saving and effective way to construct hierarchical zeolites,which may gain wide applications in fine chemical manufacturing.

关键词： Hierarchical NaX zeolite Template-free synthesis Natural kaolinite Knoevenagel condensation

Thermoelectric Properties of an Indandione-Terminated Quinoidal Compound:Effect of the n-Type Dopants

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Chinese Journal of Chemistry 2024年第9期42卷 997-1003页

作者： Yingying Liu Cheng wang Tianzuo wang Fei Jiao Shaoqiang Dong Yunfeng Deng Yanhou Geng School of Materials Science and Engineering and Tianjin Key Laboratory of Molecular Optoelectronic Science Tianjin Universityand Collaborative Innovation Center of Chemical Science and Engineering(Tianjin)Tianjin 300072China Institute of Molecular Aggregation Science Tianjin UniversityTianjin 300072China Tianjin Key Laboratory of Molecular Optoelectronic Science Department of ChemistrySchoolof ScienceTianjin UniversityTianjin300072China Joint Schoolof NationalUniversity of Singapore and Tianjin University International Campus of Tianjin UniversityBinhai New City FuzhouFujian350207China

The investigation of n-type doping holds a significant interest for the application of ***,the doping of an indandione-terminated compound Q-4F with a singlet open-shell ground state was studied using two n-dopants N-DMBI and *** of these two dopants can effectively dope Q-4F due to the large offset between the singly occupied molecular orbital(SOMO)of dopants and the lowest unoccupied molecular orbital(LUMO)of Q-4F.N-DMBI has a higher doping ability than LCV as demonstrated by the UV-vis-NIR and EPR ***,in comparison to N-DMBI doped Q-4F,LCV doped system exhibits much higher electrical conductivity and power factor due to its unperturbed molecular packing and favorable morphology after *** optimal conductivity of LCV doped Q-4F is 7.16×10^(-2)±0.16 S·cm^(-1) and the highest power factor reaches 12.3±0.85μW·m–1·K^(-2).These results demonstrate that the modulation of n-dopants is a powerful strategy to balance the doping efficiency and microstructure toward a maximum thermoelectric performance.

关键词： n-Doping Indandione Quinoidal compounds Organic thermoelectrics Electron transfer Organic electronics Energy conversion

Bilayer separator enabling dendrite-free zinc anode with ultralong lifespan >5000 h

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Green Energy & Environment 2024年第4期9卷 771-776页

作者： Lu wang Feifei wang Zhe Ding Yingxin Liu Ziyi Zhang Chunpeng Yang Kian Ping Loh Quan-Hong Yang Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityFuzhou350207China Nanoyang Group State Key Laboratory of Chemical EngineeringSchool of Chemical Engineering and TechnologyTianjin UniversityCollaborative Innovation Center of Chemical Science and Engineering(Tianjin)Tianjin300072China Haihe Laboratory of Sustainable Chemical Transformations Tianjin300192China Department of Chemistry National University of Singapore117543Singapore Institute of Process Engineering Chinese Academy of SciencesBeijing100190China

Aqueous zinc(Zn)batteries with Zn metal anodes are promising clean energy storage devices with intrinsic safety and low ***,Zn dendrite growth severely restricts the use of Zn *** effectively suppress Zn dendrite growth,we propose a bilayer separator consisting of commercial butter paper and glassfiber *** dense cellulose-based butter paper(BP)with low zincophilicity and high mechanical properties prevents the pore-filling behavior of deposited Zn and related separator piercing,effectively suppressing the Zn dendrite *** a result,the bilayer separators endow the ZnjjZn symmetrical batteries with a superlong cycling life of Zn anodes(over 5000 h)at 0.5 mA cm^(-2) and the full batteries enhanced capacity retention,demonstrating the advancement of the bilayer separator to afford excellent cyclability of aqueous metal batteries.

关键词： Zn battery Bilayer separator Butter paper Zn metal anode Zn dendrite

Density functional theory for adsorption of HCHO on the FeO(100) surface

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Journal of Natural Gas Chemistry 2010年第1期19卷 21-24页

作者： Lingling wang, Wenkai Chen Department of Chemistry, fuzhou University, fuzhou 350108, Fujian, China Department of Chemistry Fuzhou University Fuzhou 350108 Fujian China

The density functional theory （DFT） and periodic slab model were used to get information concerning the adsorption of HCHO on the FeO（100） surface. A preferred η^2-（C,O）-di-σ four-membered ring adsorption conformation on the Fe-top site was found to be the most favorable structure with the predicted adsorption energy of 210.7 kJ/mol. The analysis of density of states, Mulliken population, and vibrational frequencies before and after adsorption showed clear weakening of the carbonyl bond, and high sp^3 character on the carbon atom.

关键词： density functional theory formaldehyde iron monoxide adsorption