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Geochemical characteristics,generation,and evolution mechanism of coalbed methane in the south-western Ordos Basin,China

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Frontiers of Earth Science 2024年第2期18卷 296-311页

作者： Yabing LIN Yong QIN Dongmin MA Shengquan WANG College of Geology and Environment Xi’an University of Science and TechnologyXi’an 710054China key laboratory of Coalbed Methane resource and reservoir Formation process(the Ministry of Education) China University of Mining and TechnologyXuzhou 221008China Shaanxi Provincial key laboratory of Geological Support for Coal Green Exploitation Xi’an 710054China

The south-western Ordos Basin is rich in low-middle rank coalbed methane(cbm)resources;while the geochemical characteristics and genetic mechanism of cbm are not ***,according to geological and geochemical test data from gas and coal seam water from cbm wells in Bingchang,Jiaoxun,Huangling,Yonglong,and Longdong minging areas,we systematically studied the geochemical characteristics,generation,and evolution mechanism of cbm in Jurassic Yan’an Formation in the south-western Ordos *** results show that the CH4 content of whole gas is in the range of 42.01%-94.72%.The distribution ranges of theδ^(13)C-CH_(4)value is−87.2‰to−32.5‰,indicating diverse sources of thermogenic gas and biogenic *** microbial methane is mainly generated by a CO_(2)reduction pathway,with certain methyl-type fermentation ***δ^(13)C-CH_(4)has a positive correlation with burial depth,indicating the obvious fractionation of *** relationship between the genetic types and burial depth of the cbm reservoir indicates that the favorable depth of secondary biogenic gas is less than 660 *** Late Cretaceous Yanshanian Movement led to the uplift of the Ordos Basin,and a large amount of thermogenic gas escaped from the edge of the *** the Paleogene Period,the coal reservoir in the basin margin has received recharge from atmospheric precipitation,which is favorable for the formation of secondary biogenic *** deep area,generally under 1000 m,mainly contains residual thermogenic *** intermediate transition zone is mixed *** by the tectonic background,the genetic types of cbm in different mining areas are controlled by the coupling of burial depth,coal rank,and hydrogeological *** Binchang mining area contains biogenic gas,and the development of cbm has achieved initial success,indicating that similar blocks with biogenic gas formation conditions is key to the efficient development of *** research results provide a scientific basis for

关键词： coalbed methane stable isotopes geochemistry generation and evolution mechanism Ordos Basin

Ligand effect in surface atomic sites of group VI B transition metals on ultrathin Pt nanowires for enhanced oxygen reduction

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Nano Research 2024年第6期17卷 5298-5304页

作者： Yuwei He Yueguang Chen Renjie Wu Zhihe Xiao Mengxian Li Chunfeng Shi Leyu Wang State key laboratory of Chemical resource Engineering College of ChemistryBeijing University of Chemical TechnologyBeijing 100029China State key laboratory of Petroleum Molecular and process Engineering SINOPEC Research Institute of Petroleum Processing Co.Beijing 100083China

Increasing the utilization efficiency of platinum is critical for advancing proton exchange-membrane fuel cells(PEMFCs).Despite extensive research on catalysts for the cathodic oxygen reduction reaction(ORR),developing highly active and durable Pt-based catalysts that can suppress surface dealloying in corrosive acid conditions remains ***,we report a facile synthesis of bimetallic ultrathin PtM(M=Mo,W,and Cr)nanowires(NWs)composed of group VI B transition metal atomic sites anchored on the *** NWs possess uniform sizes and well-controlled atomic *** to PtW and PtCr catalysts,the PtMo0.05 NWs exhibit the highest half-wave potential of 0.935 V and a mass activity of 1.43 A·mgPt^(−1).Remarkably,they demonstrate a remarkable 23.8-fold enhancement in mass activity compared to commercial Pt/C for ORR,surpassing previously reported Pt-based ***,the PtMo NWs cathode in membrane electrode assembly tests achieves a remarkable peak power density of 1.443 W·cm^(−2)(H_(2)-O_(2)conditions at 80℃),which is 1.09 times that of commercial Pt/*** ligand effect in the bimetallic surface not only facilitates strong coupling between Mo(4d)and Pt(5d)atomic orbitals to hinder atom leaching but also modulates the d-states of active site,significantly optimizing the adsorption of key oxygen(*O and*OH)species and accelerating the rate-determining step in ORR pathways.

关键词： ligand effect oxygen reduction reaction group VI B transition metal ultrathin nanowires multiple oxygen species

Solvent effects on Diels-Alder reaction in ionic liquids:A reaction density functional study

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Chinese Journal of Chemical Engineering 2024年第2期66卷 180-188页

作者： Zijiang Dou Weiqiang Tang Peng Xie Shuangliang Zhao Guangxi key laboratory of Petrochemical resource processing and process Intensification Technology and School of Chemistry and Chemical Engineering Guangxi UniversityNanning 530004China State key laboratory of Chemical Engineering and School of Chemical Engineering East China University of Science and TechnologyShanghai 200237China

Extensive experimental studies have been performed on the Diels-Alder(DA)reactions in ionic liquids(ILs),which demonstrate that the IL environment can significantly influence the reaction rates and ***,the underlying microscopic mechanism remains *** this work,the multiscale reaction density functional theory is applied to explore the effect of 1-butyl-3-methylimidazolium hexafluorophosphate([BMIM][PF_(6)])solvent on the reaction of cyclopentadiene(CP)with acrolein,methyl acrylate,or *** analyzing the free energy landscape during the reaction,it is found that the polarization effect has a relatively small influence,while the solvation effect makes both the activation free energy and reaction free energy *** addition,the rearrangement of local solvent structure shows that the cation spatial distribution responds more evidently to the reaction than the anion,and this indicates that the cation plays a dominant role in the solvation effect and so as to affect the reaction rates and selectivity of the DA reactions.

关键词： Solvent effect Ionic liquids Diels-Alder reaction Reaction density functional theory

Controlling solid form and crystal habit of triphenylmethanol by antisolvent crystallization in a microfluidic device

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Chinese Chemical Letters 2024年第4期35卷 393-398页

作者： Jun Lu Jinrui Yan Yaohao Guo Junjie Qiu Shuangliang Zhao Bo Bao East China University of Science and Technology Shanghai 200237China Guangxi key laboratory of Petrochemical resource processing and process Intensification Technology and School of Chemistry and Chemical Engineering Guangxi UniversityNanning 530004China

Crystal habit and crystal form are critical elements in determining product properties and functions. In this work, we developed a microfluidic antisolvent crystallization technique to rapidly screen and accurately control the solid form and crystal habit of triphenylmethanol(Ph_(3)COH). This advanced technique separates the primary mixing of solutions from crystal formation(nucleation and growth) by introducing the microfluidic device, avoiding clogging in microchannels to obtain high-quality crystals. The results show that we can achieve controllable preparation of pure 2Ph_(3)COH·DMSO(DMSO solvate), pure Ph_(3)COH(form β), and mixed crystals with different mass ratios. Moreover, the microscale can prompt the DMSO solvate to grow into hexagonal sheet-like and bulk crystals. We can regulate the aspect ratio of hexagonal sheet-like crystals in binary solvents and control the crystal habit of the form β to transition between long needle-like shapes and short hexagonal prisms in DMF-H_(2)O. Meanwhile, we revealed that the solvent ratio, the antisolvent flow rate, and the initial concentration of Ph_(3)COH are the main factors affecting the solid form selectivity and morphology transition. Such a novel method would be considered as a promising technique to be extended to screen and control key crystallization parameters of other substances.

关键词： Microfluidics Triphenylmethanol Antisolvent crystallization Crystal habit Solid form

Controllable chemical redox reactions to couple microbial degradation for organic contaminated sites remediation:A review

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Journal of Environmental Sciences 2024年第5期139卷 428-445页

作者： Bin Chen Jiang Xu Lizhong Zhu College of Environmental and resource Sciences Zhejiang UniversityHangzhou 310058China Zhejiang Provincial key laboratory of Organic Pollution process and Control Zhejiang UniversityHangzhou 310058China Zhejiang Agriculture&Forest University Lin'an 311300China

Global environmental concern over organic contaminated sites has been progressively conspicuous during the process of urbanization and industrial *** traditional physical or chemical remediation technologies may significantly destroy the soil structure and function,coupling moderate chemical degradation with microbial remediation becomes a potential way for the green,economic,and efficient remediation of contaminated ***,this work systematically elucidates why and how to couple chemical technology with microbial remediation,mainly focused on the controllable redox reactions of organic *** rational design of materials structure,selective generation of reactive oxygen species,and estimation of degradation pathway are described for chemical ***,current progress on efficient and selective reductions of organic contaminants(i.e.,dechlorination,defluorination,-NO_(2) reduction)is *** with the microbial remediation of contaminated sites,several consideration factors of how to couple chemical and microbial remediation are proposed based on both fundamental and practical points of *** review will advance the understanding and development of chemical-microbial coupled remediation for organic contaminated sites.

关键词： Soil remediation Groundwater remediation Rational design Reactive species Environmental nanotechnology

Micro-sized nanoaggregates:Spray-drying-assisted fabrication and applications

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Particuology 2024年第2期85卷 22-48页

作者： Dan-Lei Yang Rong-Kun Liu Yan Wei Qian Sun Jie-Xin Wang School of Life Sciences and Chemical Engineering Jiangsu Second Normal UniversityNanjing210013China State key laboratory of Organic-Inorganic Composites Beijing University of Chemical TechnologyBeijing100029China Guangxi key laboratory of Petrochemical resource processing and process Intensification Technology School of Chemistry and Chemical EngineeringGuangxi UniversityNanning530004China

The applications of nanoparticles suffer from their extremely small size and intrinsic trend of *** nanoparticles to form micro-sized nanoaggregates(MNAs)with increased size,ordered structure,as well as controllable size,shape,and morphology is a crucial step in various fields of science and technology to maintain the unique characteristics of nanoparticles while obtaining greatly enhanced or new performance at the *** structure of MNAs prominently affects their functionality,which is determined by the arrangement of nanoparticles and the interaction between primary *** methods have been proposed to prepare the MNAs,in which spray-drying technology stands out considering the feasibility,scalability for industry,cost,and *** assembly of nanoparticles through spray-drying under tunable process parameters yields diverse physical properties and structural arrangements of nanoparticles of the MNAs,they therefore exhibit enormous potential in a wide range of application *** review presents the construction and applications of spray-dried *** factors that influence the size,morphology,and structure of the MNAs are discussed in *** addition,the outstanding application performance resulting from the tightly packed nanoparticles in regular-shaped MNAs obtained by the spray-drying process is illustrated.

关键词： Spray-drying Micro-sized nanoaggregates Applications

Efficient piezo-assisted near-infrared-light-driven Cr（Ⅵ） reduction over Bi2S3 nanowires transformed from ultrathin Bi2WO6 nanosheets

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Rare Metals 2024年第9期43卷 4333-4343页

作者： Qiang Zhang Yuan-Hao Cheng Wei Liu Hui-Nan Che Yan-Hui Ao key laboratory of Integrated Regulation and resource Development On Shallow Lakes Ministry of Education College of Environment Hohai University

The utilization of piezo-photocatalytic technol ogy for environmental remediation under full spectrum solar light is promising but still ***,one dimensional Bi2S3nanowires,which can utilize both mechanical energy and near-infrared （NIR） light to remov hexavalent chromium (Cr （VI）) efficiently,were synthe sized by a restrained growth *** reaction rat constants of Cr （VI） reduction in piezo-photocatalyti process under NIR （800–2500 nm） reached 0.334 min-1which were 3.2 and 12.4 times as that of single piezo and photocatalytic *** formation of polarized electri fields and one-dimensional structure allow ultrafast sepa ration of charge carriers,thereby promoting the catalyti ***,due to the strong penetrability o NIR light,the piezo-photocatalysis performance in turbid solutions under NIR light (0.188 min-1) was even com parable to that under visible light (0.186 min-1).Thi study provides a new concept on the development of piezo photocatalytic technology for environmental remediation by utilization of NIR light and natural mechanical energy

关键词： Bi2S3 nanowires Cr(VI) NIR light Piezo-photocatalysis

NIR-Ⅱ responsive Janus nanoparticles amplify immunogenic cell death for enhanced cancer immunotherapy

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Science China(Technological Sciences) 2024年第1期67卷 321-329页

作者： CHEN BeiBei GUO KangLi WANG HaoRan XU Fu-Jian WANG JuLin ZHAO NaNa State key laboratory of Chemical resource Engineering Beijing University of Chemical TechnologyBeijing 100029China key laboratory of Biomedical Materials of Natural Macromolecules(Beijing University of Chemical Technology) Beijing Laboratory of Biomedical MaterialsBeijing University of Chemical TechnologyBeijing 100029China College of Materials Sciences and Engineering Beijing University of Chemical TechnologyBeijing 100029China Beijing key laboratory of Electrochemical process and Technology for Materials Beijing University of Chemical TechnologyBeijing 100029China

Immunotherapy brings new hope for tumor treatment by inducing immunogenic cell death(ICD)of tumor ***,insufficient immunogenicity and low immune response rate greatly limit antitumor ***,by optimizing the composition and morphology,the rational design of Janus nanoparticles composed of Fe_(3)O_(4) nanospheres and SiO_(2)nanorods was realized for enhanced cancer immunotherapy through amplified *** glucose oxidase(GOx)was loaded by the Janus nanoparticles,the resultant M-FS-GOx consumes glucose at tumor sites to generate gluconic acid and hydrogen peroxide(H_(2)O_(2))for starvation therapy while the H_(2)O_(2)supply promotes the production of highly toxic·OH to achieve effective chemodynamic therapy(CDT).Under a 1064 nm light irradiation,the photothermal effect of M-FS-GOx enhances the enzyme activity of GOx for improved starvation ***,both tumor-associated antigens released during the process of ICD and the intrinsic immunoadjuvant property of M-FS-GOx stimulate dendritic cell maturation to activate antitumor immune *** work provides a promising strategy for the construction of Janus nanoparticles to achieve enhanced cancer immunotherapy through combination therapy-amplified ICD.

关键词： Janus nanoparticles immunogenic cell death cancer immunotherapy

Role of catalyst surface-active sites in the hydrogenation ofα,β-unsaturated aldehyde

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Frontiers of Chemical Science and Engineering 2024年第6期18卷 41-69页

作者： Haixiang Shi Tongming Su Zuzeng Qin Hongbing Ji School of Chemistry and Chemical Engineering Guangxi Key Laboratory of Petrochemical Resource Processing and Process Intensification TechnologyGuangxi UniversityNanning 530004China Zhejiang Green Petrochemical and Light Hydrocarbon Transformation Research Institute Zhejiang University of TechnologyHangzhou 310014China

As an important technology in fine chemical production,the selective hydrogenation ofα,β-unsaturated aldehydes has attracted much attention in recent *** the process ofα,β-unsaturated aldehyde hydrogenation,a conjugated system is formed between>C=CC=O,leading to hydrogenation at both ends of the conjugated system,which competes with each other and results in more complex ***,improving the reaction selectivity is also difficult in industrial ***,many researchers have reported that surface-active sites on catalysts play a crucial role inα,β-unsaturated aldehyde *** review attempts to summarize recent advances in understanding the effects of surface-active sites(SASs)over metal catalysts for enhancing the process of *** construction strategies and roles of SASs for hydrogenation catalysts are *** attention has been given to the adsorption configuration and transformation mechanism ofα,β-unsaturated aldehydes on catalysts,which contributes to understanding the relationship between SASs and hydrogenation *** addition,recent advances in metal-supported catalysts for the selective hydrogenation ofα,β-unsaturated aldehydes to understand the role of SASs in hydrogenation are briefly ***,the opportunities and challenges will be highlighted for the future development of the precise construction of SASs.

关键词： α,β-unsaturatedd aldehydes hydrogenation active site cinnamaldehyde