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Energy transfer enhanced photocatalytic hydrogen evolution in organic heterostructure nanoparticles via flash nanoprecipitation processing

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Green Energy & Environment 2025年第2期10卷 390-398页

作者： Miaojie Yu Weiwei Zhang Xueyan Liu Guohui Zhao Jun Du Yongzhen Wu Wei-Hong Zhu key laboratory for Advanced Materials and Institute of Fine Chemicals Joint International Research Laboratory of Precision Chemistry and Molecular EngineeringFeringa Nobel Prize Scientist Joint Research CenterFrontiers Science Center for Materiobiology and Dynamic ChemistrySchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai200237China state key laboratory of molecular reaction dynamics Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalianLiaoning116023China

Organic nanophotocatalysts are promising candidates for solar fuels production,but they still face the challenge of unfavorable geminate recombination due to the limited exciton diffusion ***,we introduce a binary nanophotocatalyst fabricated by blending two polymers,PS-PEG5(PS)and PBT-PEG5(PBT),with matched absorption and emission spectra,enabling a F€orster resonance energy transfer(FRET)process for enhanced *** heterostructure nanophotocatalysts are processed using a facile and scalable flash nanoprecipitation(FNP)technique with precious kinetic control over binary nanoparticle *** resulting nanoparticles exhibit an exceptional photocatalytic hydrogen evolution rate up to 65 mmol g^(-1) h^(-1),2.5 times higher than that single component *** through fluorescence spectra and transient absorption spectra confirm the hetero-energy transfer within the binary nanoparticles,which prolongs the excited-state lifetime and extends the namely“effective exciton diffusion length”.Our finding opens new avenues for designing efficient organic photocatalysts by improving exciton migration.

关键词： Polymer photocatalysts Nanoparticles Hydrogen evolution F€orster resonance energy transfer

A New Diabatic Potential Energy Matrix for the Two Lowest Electronic states of H3

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Chinese Journal of Chemical Physics 2025年第1期38卷 37-44,I0055页

作者： Yingyue Hong Yafu Guan Dong H.Zhang state key laboratory of molecular reaction dynamics Dalian Institute of Chemical PhysicsChinese Academy of ScienceDalian 116023China School of Chemical Sciences University of Chinese Academy of SciencesBeijing 100049China

A new two-state diabatic potential energy matrix(DPEM)for H3 has been constructed,based on the fun-damental invariant neural network(FI-NN)diabatization method pro-posed in our previous work[***.21,15040(2019)].In that initial effort,a two-state DPEM was constructed only with a 10 eV energy *** current work aims to expand the en-ergy range and improve the accura-cy of *** is achieved by the utilization of full configuration inter-action(FCI)with aug-cc-pVnZ ba-sis sets and complete basis set(CBS)*** original dataset is augmented with additional points with higher adiabatic energies,which give rise to a total of 10985 data *** DPEM constructed in this work now enables accurate representation of adiabatic energies up to 18 *** dynamic calculations based on this DPEM are nearly identical to those obtained from benchmark surfaces,which makes it the most accurate DPEM for the H3 system to date,therefore facilitating detailed exploration of reaction mechanisms at higher collision energies.

关键词： Diabatic potential energy matrix Conical intersection Fundamental invariant neural network

Synergistic enhancement of ion/electron transport by ultrafine nanoparticles and graphene in Li2FeTiO4/C/G nanofibers for symmetric Li-ion batteries

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Journal of Energy Chemistry 2025年第02期101卷 42-51页

作者： Wenjie Ma Yakun Tang Yue Zhang Xiaohui Li Lang Liu Xueting Wang Yuliang Cao state key laboratory of Chemistry and Utilization of Carbon Based Energy Resources Key Laboratory of Energy Materials Chemistry Ministry of Education College of Chemistry Xinjiang University College of Chemistry and molecular Sciences Hubei Key Laboratory of Electrochemical Power Sources Wuhan University

Low-cost Fe-based disordered rock salt（DRX） Li2FeTiO4is capable of providing high capacity(295 mA h g-1) by redox activity of cations(Fe2+/Fe4+and Ti3+/Ti4+) and anionic ***,DRX structures lack transport channels for ions and electrons,resulting in sluggish kinetics,poor electrochemical activity,and ***,graphene conductive carbon network permeated Li2FeTiO4（LFT/C/G） nanofibers are successfully prepared by a facile sol-gel assisted electrospinning *** Li2FeTiO4nanoparticles（2 nm） and one-dimensional（1D） structure provide abu ndant active sites and unobstructed diffu sion channels,accelerating ion *** addition,introducing graphene reduces the band gap and Li+diffusion barrier and improves the dynamic properties of Li2FeTiO4,thus achieving a relatively mild interfacial reaction and reversible redox *** expected,the LFT/C/1.0G cathode delivers a remarkable discharge capacity(238.5 mA h g-1),high energy density(508.8 Wh kg-1),and excellent rate capability(51.2 mA hg-1at 1.0 A g-1).Besides,the LFT/C/1.0G anode also displays a high capacity(514.5 mA h g-1at 500 mA g-1) and a remarkable rate capability(243.9 mA h g-1at 8 A g-1).Moreover,the full batteries based on the LFT/C/1.0G symmetric electrode demonstrate a reversible capacity of 117.0 mA h g-1after 100 cycles at 50 mA *** study presents useful insights into developing cost-effective DRX cathodes with durable and fast lithium storage.

关键词： 1D structure Disordered rock salt Li2FeTiO4 Graphene Lithium-ion battery electrode Rapid ion/electron transport

Classification and progress of extraction technologies for nonferrous metal resources

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Science China Chemistry 2025年第2期68卷 458-474页

作者： Fangqin Cheng Na Zhou Nazeer Muhammad Nouman Li Cui Caixia Yin Institute of Resources and Environmental Engineering State Environmental Protection Key Laboratory of Efficient Utilization of Coal Waste ResourcesShanxi UniversityTaiyuan 030006China key laboratory of Chemical Biology and molecular Engineering of Ministry of Education Institute of Molecular ScienceShanxi UniversityTaiyuan 030006China

In recent years,the demand for strategic metal resources,essential for scientific and technological progress and industrial development,has *** a stable supply of these metals is critical to national security and the well-being of the *** global industrialization accelerates,the daily demand for nonferrous metals continues to ***,extracting and recovering strategic metals from low-grade raw materials,such as solid waste,has become crucial for maintaining their supply and economic ***,the extraction process is fraught with challenges,including mineral phase stability and complex *** review focuses on key strategic metals such as lithium,aluminum,gallium,and *** introduces and examines various methods for extracting nonferrous metals from different raw materials,including traditional mining technologies applied to low-grade solid *** also outlines future development opportunities and challenges in this field.

关键词： nonferrous metal extraction classification and progress

Synthesis of ordered mesoporous crystalline boron phosphate scaffold with double diamond surface structure

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Science China Chemistry 2025年第2期68卷 590-600页

作者： Chao Wang Wen-Duo Lu Jiao Wang Shunai Che An-Hui Lu Lu Han School of Chemical Science and Engineering Tongji UniversityShanghai 200092China state key laboratory of Fine Chemicals Liaoning Key Laboratory for Catalytic Conversion of Carbon ResourcesSchool of Chemical EngineeringDalian University of TechnologyDalian 116024China School of Chemistry and Chemical Engineering Frontiers Science Center for Transformative MoleculesState Key Laboratory of Metal Matrix CompositesShanghai Key Laboratory for Molecular Engineering of Chiral DrugsShanghai Jiao Tong UniversityShanghai 200240China

Ordered mesoporous materials have received great attention due to their well-defined pore structures and potential applications in catalysis,adsorption,separation,drug delivery,*** various compositions of mesoporous solids have been successfully prepared,the preparation of crystalline non-metallic oxyacid salts with ordered mesoporosity remains a major ***,we report the synthesis of a mesoporous solid acid crystalline boron phosphate(BPO_(4))catalyst with a bicontinuous shifted double diamond(SDD)hyperbolic surface *** BPO_(4) scaffold was obtained by synergistic selfassembly in a mixed solvent of water and tetrahydrofuran using the diblock copolymer poly(ethylene oxide)-block-polystyrene as template and phosphoric acid and orthoboric acid as inorganic *** structure consists of two sets of diamond networks adjacent to each other with a mesostructural scale tetragonal symmetry(space group I4_(1)/amd)with unit cell parameters of a=80 nm and c=113 nm,which affords the scaffold a specific surface area of 44 m^(2)/*** a solid acid catalytic material,the SDD BPO_(4) scaffold exhibited excellent catalytic activity at room temperature with a conversion of furfural to 2-(dimethoxymethyl)furan over 70%and can be reused after recovery without serious loss of *** the propane oxidative dehydrogenation reaction,SDD BPO_(4) demonstrated high olefin productivity and selectivity while maintaining high reaction *** study provides ideas for the preparation of ordered mesoporous crystalline catalytic materials and demonstrates their potential for practical applications.

关键词： boron phosphate mesoporous material self-assembly block copolymer catalyst

Recent progress on photoactive nonprecious transition-metal complexes

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Science China Chemistry 2025年第1期68卷 46-95页

作者： Zhong-Liang Gong Hong-Jie Zhang Yan Cheng Jianxun Liu Yuhan Ai Yaqin Li Zhihui Feng Qiong Zhang Shaolong Gong Yong Chen Chang-Jiang Yao Yuan-Yuan Zhu Liang-Jin Xu Yu-Wu Zhong CAS key laboratory of Photochemistry Institute of ChemistryChinese Academy of SciencesBeijing 100190China state key laboratory of Structural Cemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China School of Chemistry and Chemical Engineering Anhui Key Laboratory of Advanced Catalytic Materials and Reaction EngineeringHefei University of TechnologyHefei 230009China state key laboratory of Explosion Science and Safety Protection School of Mechatronical EngineeringBeijing Institute of TechnologyBeijing 100081China College of Chemistry and molecular Sciences Hubei Key Lab on Organic and Polymeric Optoelectronic MaterialsWuhan UniversityWuhan 430072China School of Chemistry and Chemical Engineering Anhui UniversityHefei 230601China key laboratory of Photochemical Conversion and Optoelectronic Materials&CAS-HKU Joint laboratory on New Materials Technical Institute of Physics and ChemistryChinese Academy of SciencesBeijing 100190China

Photoactive complexes of nonprecious transition metals,mainly including those in the first-row and partially the second-row of the Periodic table of elements,have received increasing attention in view of their low cost and long-term *** are recognized as promising alternatives to noble transition metal complex congeners that have been extensively studied in optoelectronic devices,artificial photosynthesis,photocatalysis,biodiagnostics,and therapeutics,*** review is devoted to a comprehensive summary on the classical and recent advances on photoactive nonprecious transition metal complexes,including photoactive Zr,V,Cr,Mo,and W complexes,Mn complexes and hybrids,Fe,Co,Ni,and Cu complexes,and Zn and Cd complexes and hybrids.A particular focus is given on the molecular design,modulation of photophysical and photochemical properties,and applications of the representative and lately-developed nonprecious metal *** addition,a perspective on the future development in this field is provided at the end of this review.

关键词： photoactive metal complexes earth-abundant metals nonprecious metal complexes luminescence photochemistry

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Upcycling of polyphenylene oxide into 2,6-dimethyl aniline via depolymerization and amination over a Pt/CeO_(2) catalyst

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Science China Chemistry 2025年第2期68卷 520-525页

作者： Shengchao Jia Wenke Zhao Xiaohui Liu Yong Guo Yanqin Wang state key laboratory of Green Chemical Engineering and Industrial Catalysis Research Institute of Industrial CatalysisSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237China Shanghai key laboratory of Functional Materials Chemistry School of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237China

Upcycling of plastic waste into N-containing compound is a novel and attractive strategy for its disposal and will opens up a promising direction for the production of value-added ***,an efficient strategy for the depolymerization-amination of polyphenylene oxide(PPO)into 2,6-dimethyl aniline is developed over a simple Pt/CeO_(2) *** C–O linkages of PPO can be selectively broken,producing 2,6-dimethyl phenol and then hydrogenated and aminated to 2,6-dimethyl cyclohexylamine over the Pt/CeO_(2) ***,2,6-dimethyl aniline was produced with high selectivity through the dehydrogenation of 2,6-dimethyl cyclohexylamine in the same *** can be used as the hydrogen-acceptor in the dehydrogenation step and enhance the selectivity of target *** N-containing compound,2,6-dimethyl aniline,is obtained and separated after HCl ***,the Pt/CeO_(2) catalyst exhibit remarkable stability and can sustainably catalyze the synthesis of 2,6-dimethyl aniline in several cycles.

关键词： PPO depolymerization-amination 2,6-dimethyl aniline Pt/CeO_(2)

Improvement of charge-transfer kinetics via MXene and cobalt containing polyoxometalate loading on CdS for photocatalytic hydrogen production

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Science China Chemistry 2025年第2期68卷 772-780页

作者： Yu Feng Xiao Fang Jinnuo Zang Bin Song Chunlian Hu Xiaoyu Dong Yong Ding state key laboratory of Applied Organic Chemistry Key Laboratory of Advanced Catalysis of Gansu ProvinceCollege of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou 730000China state key laboratory of Low Carbon Catalysis and Carbon Dioxide Utilization State Key Laboratory for Oxo Synthesis and Selective OxidationLanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou 730000China

Hydrogen is a renewable and clean energy,and photocatalytic water splitting for hydrogen evolution technology is a promising technical means to solve the development *** this study,the ternary composite Co_(8)POM@MXene–CdS hybrid catalyst was constructed and used for photocatalytic hydrogen *** the condition of AM 1.5G simulated sunlight,the photocatalytic H_(2) evolution rate of the ternary composite was 8.13 mmol g^(−1) h^(−1),which was more than 25 times higher than that of the bare *** means of synchronous illumination X-ray photoelectron spectroscopy(SI-XPS)and density functional theory(DFT)calculations,it was proved that the loading of MXene and Co_(8)POM improved the photogenerated carrier separation and immigration efficiency on *** photogenerated electrons transfer from CdS to ***_(8)POM containing the{Co_(4)O_(3)}quasi-cubane,as an oxidation co-catalyst,accepts photogenerated holes from CdS to catalyze the oxidation reaction of TEOA,which improves the photocatalytic hydrogen production activity and the stability of CdS.

关键词： CdS polyoxometalates MXene hybrid catalyst photocatalytic hydrogen evolution

Carbon Dots-Modified Hollow Mesoporous Photonic Crystal Materials for Sensitivityand Selectivity-Enhanced Sensing of Chloroform Vapor

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Nano-Micro Letters 2025年第4期17卷 381-398页

作者： Junchen Liu Ji Liu Zhipeng Li Liupeng Zhao Tianshuang Wang Xu Yan Fangmeng Liu Xiaomin Li Qin Li Peng Sun Geyu Lu Dongyuan Zhao state laboratory On Integrated Optoelectronics College of Electronic Science and EngineeringJilin UniversityChangchun 130012People’s Republic of China Department of Chemistry and laboratory of Advanced Materials Shanghai Key Laboratory of Molecular Catalysis and Innovative MaterialsState Key Laboratory of Molecular Engineering of PolymersCollaborative Innovation Center of Chemistry for Energy Materials(2011-iChEM)College of Chemistry and MaterialsFudan UniversityShanghaiPeople’s Republic of China School of Engineering and Built Environment Griffith UniversityNathanQLD 4111Australia

Chloroform and other volatile organic pollutants have garnered widespread attention from the public and researchers,because of their potential harm to the respiratory system,nervous system,skin,and ***,research on chloroform vapor sensing is still in its early stages,primarily due to the lack of specific recognition *** we report a mesoporous photonic crystal sensor incorporating carbon dots-based nanoreceptor(HMSS@CDs-PCs)for enhanced chloroform *** colloidal PC packed with hollow mesoporous silica spheres provides an interconnected ordered macro-meso-hierarchical porous structure,ideal for rapid gas sensing utilizing the photonic bandgap shift as the readout *** as-synthesized CDs with pyridinic-N-oxide functional groups adsorbed in the hollow mesoporous silica spheres are found to not only serve as the chloroform adsorption sites,but also a molecular glue that prevents crack formation in the colloidal *** sensitivity of HMSS@CDs-PCs sensor is 0.79 nm ppm^(-1)and an impressively low limit of detection is 3.22 ppm,which are the best reported values in fast-response chloroform vapor sensor without multi-signal *** positive response time is 7.5 s and the negative response time 9 ***,relatively stable sensing can be maintained within a relative humidity of 20%-85%RH and temperature of 25-55℃.This study demonstrates that HMSS@CDs-PCs sensors have practical application potential in indoor and outdoor chloroform vapor detection.

关键词： Carbon dots Photonic crystal sensors Sensitivity-enhanced sensing Selectivity-enhanced sensing Chloroform vapor sensing

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