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Activity promotion of Rh_(1)Ca_(x)/Al_(2)O_(3) single-atom catalyst in 1-octene hydroformylation:a volcano curve exists between Ca adding ratio and catalytic activity

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Science China Chemistry 2024年第4期67卷 1187-1192页

作者： Hao Zhang Xingcong Zhang Xilun Wang Qingdi Sun Hao Liu Hongbing Ji Xiaohui He Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education Fine Chemical Industry Research InstituteSchool of ChemistryIGCMESun Yat-sen UniversityGuangzhou 510275China Huizhou research institute Sun Yat-sen UniversityHuizhou 516081China State Key Laboratory Breeding Base of green-Chemical Synthesis Technology Institute of Green Petroleum Processing and Light Hydrocarbon ConversionCollege of Chemical EngineeringZhejiang University of TechnologyHangzhou 310014China

Single-atom catalysts(SACs)are considered the best candidates for olefin hydroformylation due to their combined advantages of homogeneous and heterogeneous *** conventional organo-phosphine modification,Rh SAC is modified by introducing Ca,resulting in a significant increase in activity(maximum~5.7-fold)and ***,a volcano curve between Ca addition ratio and catalytic activity is *** Ca significantly increases activity by decreasing the energy barrier,but excessive Ca decreases activity due to hindering substrate adsorption and reaction.

关键词： hydroformylation bimetallic single-atom catalysts rhodium heterogeneous catalyst

Hyperbranched polymer hollow-fiber-composite membranes for pervaporation separation of aromatic/aliphatic hydrocarbon mixtures

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Chinese Journal of Chemical Engineering 2024年第5期69卷 13-22页

作者： Tong Liu Hao Sun Xiangqiong Wang Jie Li Zhanquan Zhang Pei Wu Naixin Wang Quanfu An Beijing Key Laboratory for green Catalysis and Separation Department of Chemical EngineeringCollege of Materials Science and EngineeringBeijing University of TechnologyBeijing 100124China petrochemical research institute CNPCBeijing 102206China

The separation of aromatic/aliphatic hydrocarbon mixtures is crucial in the petrochemical *** is regarded as a promising approach for the separation of aromatic compounds from alkanes. Developing membrane materials with efficient separation performance is still the main task since the membrane should provide chemical stability, high permeation flux, and selectivity. In this study, the hyperbranched polymer(HBP) was deposited on the outer surface of a polyvinylidene fluoride(PVDF)hollow-fiber ultrafiltration membrane by a facile dip-coating method. The dip-coating rate, HBP concentration, and thermal cross-linking temperature were regulated to optimize the membrane *** obtained HBP/PVDF hollow-fiber-composite membrane had a good separation performance for aromatic/aliphatic hydrocarbon mixtures. For the 50%/50%(mass) toluene/n-heptane mixture, the permeation flux of optimized composite membranes could reach 1766 g·m^(-2)·h^(-1), with a separation factor of 4.1 at 60℃. Therefore, the HBP/PVDF hollow-fiber-composite membrane has great application prospects in the pervaporation separation of aromatic/aliphatic hydrocarbon mixtures.

关键词： Aromatic/aliphatic hydrocarbons Hyperbranched polymer Pervaporation Hollow fiber membrane Dip-coating

Activity promotion of RhCa/AlOsingle-atom catalyst in1-octene hydroformylation: a volcano curve exists between Ca adding ratio and catalytic activity

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Science China Chemistry 2024年

作者： Hao Zhang Xingcong Zhang Xilun Wang Qingdi Sun Hao Liu Hongbing Ji Xiaohui He Huizhou research institute Sun Yat-sen University Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education Fine Chemical Industry Research Institute School of Chemistry IGCME Sun Yat-sen University State Key Laboratory Breeding Base of green-Chemical Synthesis Technology Institute of Green Petroleum Processing and Light Hydrocarbon Conversion College of Chemical Engineering Zhejiang University of Technology

Single-atom catalysts(SACs) are considered the best candidates for olefin hydroformylation due to their combined advantages of homogeneous and heterogeneous catalysts. Unlike conventional organo-phosphine modification, Rh SAC is modified by introducing Ca, resulting in a significant increase in activity(maximum ～5.7-fold) and stability. Furthermore, a volcano curve between Ca addition ratio and catalytic activity is found. Introducing Ca significantly increases activity by decreasing the energy barrier, but excessive Ca decreases activity due to hindering substrate adsorption and reaction.

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Systematic engineering of BiVO_(4)photoanode for efficient photoelectrochemical water oxidation

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Carbon Energy 2024年第4期6卷 12-21页

作者： Zhiting Liang Meng Li Kai‐Hang Ye Tongxin Tang Zhan Lin Yuying Zheng Yongchao Huang Hongbing Ji Shanqing Zhang Guangzhou Key Laboratory of Clean Transportation Energy Chemistry School of Chemical Engineering and Light IndustryGuangdong University of TechnologyGuangzhouChina Chemical Engineering Guangdong Laboratory Jieyang Branch of ChemistryJieyangChina Key Laboratory for Water Quality and Conservation of the Pearl River Delta Institute of Environmental Research at Greater Bay AreaMinistry of EducationGuangzhou UniversityGuangzhouChina State Key Laboratory Breeding Base of green‐Chemical Synthesis Technology Institute of Green Petroleum Processing and Light Hydrocarbon ConversionCollege of Chemical EngineeringZhejiang University of TechnologyHangzhouChina School of Environment and Science Centre for Catalysis and Clean EnergyGriffith UniversityGold Coast CampusSouthportQueenslandAustralia

BiVO_(4)is one of the most promising photoanode materials for photoelectrochemical(PEC)solar energy conversion,but it still suffers from poor photocurrent density due to insufficient light‐harvesting efficiency(LHE),weak photogenerated charge separation efficiency(Φ_(Sep)),and low water oxidation efficiency(Φ_(OX)).Herein,we tackle these challenges of the BiVO_(4)photoanodes using systematic engineering,including catalysis engineering,bandgap engineering,and morphology *** particular,we deposit a NiCoO_(x)layer onto the BiVO_(4)photoanode as the oxygen evolution catalyst to enhance theΦ_(OX)of Fe‐g‐C_(3)N_(4)/BiVO_(4)for PEC water oxidation,and incorporate Fe‐doped graphite‐phase C_(3)N_(4)(Fe‐g‐C_(3)N_(4))into the BiVO_(4)photoanode to optimize the bandgap and surface areas to subsequently expand the light absorption range of the photoanode from 530 to 690 nm,increase the LHE andΦ_(Sep),and further improve the oxygen evolution reaction activity of the NiCoO_(x)catalytic ***,the maximum photocurrent density of the as‐prepared NiCoO_(x)/Fe‐g‐C_(3)N_(4)/BiVO_(4)is remarkably boosted from 4.6 to 7.4 mA cm^(−2).This work suggests that the proposed systematic engineering strategy is exceptionally promising for improving LHE,Φ_(Sep),andΦ_(OX)of BiVO_(4)‐based photoanodes,which will substantially benefit the design,preparation,and large‐scale application of next‐generation high‐performance photoanodes.

关键词： bismuth vanadate carbon nitride charge separation heterojunction water oxidation

Controlling hydrogenation of C=C and C=O bonds in cinnamaldehyde using Pt_(1)/Ni and Pt_(1)/Co single-atom alloy catalysts

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Rare Metals 2024年第6期43卷 2859-2868页

作者： Huan-Shi Lan Yi-Da Yang Qing-Di Sun Hao Zhang Ying Zhang Qian He Ran Chen Guo-Yi Bai Xiao-Hui He Hong-Bing Ji School of Chemistry and Chemical Engineering Guangxi UniversityNanning 530004China Key Laboratory of Bioinorganicand Synthetic Chemistry of Ministry of Education Fine Chemical Industry Research InstituteSchool of ChemistryIGCMESun Yat-sen UniversityGuangzhou510275China UBFC CNRSENSMMFEMTO-ST Institute25030 Besancon CEDEXFrance College of Chemistry and Materials Science Hebei UniversityBaoding 071002China State Key Laboratory Breeding Base of green-Chemical Synthesis Technology Institute of Green Petroleum Processing and Light Hydrocarbon ConversionCollege of Chemical EngineeringZhejiang University of TechnologyHangzhou 310014China

Selective hydrogenation of C=C and C=O bonds in cinnamaldehyde(CAL)to produce desired products is a challenging task due to the complex conjugate system of the two unsaturated functional *** this study,a simple ball milling method is presented for synthesizing Pt-based single-atom alloy catalysts(SAAs)that can function as a control switch for the selective hydrogenation of CAL into highly valuable products.

关键词： alloy hydrogenation conjugate

Construction of ZnO@CDs@Co_(3)O_(4) sandwich heterostructure with multi-interfacial electron-transfer toward enhanced photocatalytic CO_(2) reduction

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Chinese Chemical Letters 2024年第4期35卷 147-152页

作者： Xiuzheng Deng Yi Ke Jiawen Ding Yingtang Zhou Hui Huang Qian Liang Zhenhui Kang Advanced Catalysis and green Manufacturing Collaborative Innovation Center CNPC-CZU Innovation AllianceSchool of Petrochemical EngineeringChangzhou UniversityChangzhou 213164China institute of Functional Nano&Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials&DevicesSoochow UniversitySuzhou 215123China zhejiang Key Laboratory of petrochemical Environmental Pollution Control National Engineering Research Center for Marine AquacultureMarine Science and Technology CollegeZhejiang Ocean UniversityZhoushan 316004China

Photocatalytic conversion of CO_(2) into small-molecule chemical feedstocks can meet the growing demand for energy and alleviate the global warming. Herein, a p-n ZnO@CDs@Co_(3)O_(4) heterojunction with sandwich structure was constructed by calcination method of self-assembled ZIF-8@CDs@ZIF-67. The ZnO@CDs@Co_(3)O_(4) with well-defined interfacial structure exhibited the significantly enhanced photocatalytic CO_(2) reduction activity, and the optimal catalyst indicated the(CO + CH_(4)) evolution rate of 214.53μmol g^(-1)h^(-1) under simulated solar light, which was superior to ZnO, Co_(3)O_(4) and binary ZnO@Co_(3)O_(4).The internal cavity, exposed active sites, multiple interfaces and constructed p-n heterojunction can facilitate the light harvesting and photoexcited electron transfer. Besides, after introduction of CDs placed in the middle layer between ZnO and Co_(3)O_(4), CDs with excellent photoelectric property further promoted charge separation and migration. This work represents an appealing strategy to construct well-defined photocatalysts for boosting CO_(2) photoreduction.

关键词： Metal-organic framework Photocatalytic CO_(2) reduction Carbon dots p-n heterojunction Sandwich heterostructure

Gas source of the Middle Jurassic Shaximiao Formation in the Zhongjiang large gas field of Western Sichuan Depression:Constraints from geochemical characteristics of light hydrocarbons

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Energy Geoscience 2024年第2期5卷 141-151页

作者： Xiaoqi Wu Jun Yang Ping Wang Huaji Li Yingbin Chen Chunhua Ni Huasheng Zeng Wuxi research institute of Petroleum Geology Petroleum Exploration and Production Research InstituteSINOPECWuxi214126China Key Laboratory of hydrocarbon Accumulation SINOPECWuxi214126China No.3 Gas Production Plant Southwest Petroleum BranchSINOPECDeyang618000China

The Zhongjiang gas field is a typical large gas field in terrigenous strata of the Western Sichuan *** remains debatable which member of the Upper Triassic Xujiahe Formation served as the source rocks and how significant the member contributed to the gas accumulations in the Zhongjiang gas *** this study,we analyzed the essential characteristics of the Lower Jurassic source rocks and the geochemical features of light hydrocarbons in natural gas from the 2nd(T3χ^(2))and 4th members(T3χ^(4))of the Upper Triassic Xujiahe Formation(T3χ),as well as the Middle Jurassic Shaximiao(J2s)and Qianfoya(J2q)*** on this,we explored the sources of the natural gas in the Zhongjiang gas field and determined the natural gas migration patterns and their effects on the properties of light hydrocarbons in the natural *** results indicate that the Lower Jurassic lacustrine source rocks of the Zhongjiang gas field contain humic organic matter,with vitrinite reflectance(R_(0))values ranging from 0.86%to 0.98%.Samples meeting the criterion for effective source rocks[total organic carbon(TOC)content≥0.75%]exhibited an average TOC content of merely 1.02%,suggesting significantly lower hydrocarbon generation potential than source rocks in the underlying T3x,which show higher thermal maturity and TOC *** natural gas samples from T3χ^(2),T3χ^(4),J2s,and J2q reservoirs,their C_(5-7)iso-alkane content was significantly higher than their n-alkane content,and their methylcyclohexane(MCH)index ranged from 59.0%to 77.3%,indicating the predominance of methylcyclohexane in C_(7)light *** indicated by the origin identification and gas-source correlation based on the geochemical features of light hydrocarbons,the natural gas in the Zhongjiang gas field is typical coal-derived *** gas from the primary pay zone of the Shaximiao Formation,with significantly high K_(1),(P_(2)+N_(2))/C_(7),and P_(3)/C_(7)values,predominantly originated from the 5th member

关键词： Zhongjiang gas field Source rock Origin of natural gas light hydrocarbon geochemistry Natural gas migration

Photoinduced transposed Paternò-Büchi reaction for effective synthesis of high-performance jet fuel

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Chinese Journal of Chemical Engineering 2024年第3期67卷 39-48页

作者： Jinxiu Hu Xianlong Liu Yi Liu Kang Xue Chengxiang Shi Xiangwen Zhang Li Wang Ji-Jun Zou Lun Pan Key Laboratory for green Chemical Technology of the Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China Haihe Laboratory of Sustainable Chemical transformations Tianjin 300192China zhejiang institute of Tianjin University Ningbo 315201China Collaborative Innovative Center of Chemical Science and Engineering(Tianjin) Tianjin 300072China

High-energy-density fuels are important for volume-limited aerospace vehicles,but the increase in fuel energy density always leads to poor cryogenic ***,we investigated the transposed Paternò-Büchi reaction of biomass cyclic ketone and cyclic alkene to synthesize a new kind of alkyl-substituted polycyclic hydrocarbon fuel with high energy density and good cryogenic *** triplet-energy-quenching results and phosphorescent emission spectra reveal the sensitization mechanism of the reaction,including photosensitizer excitation,triplettriplet energy transfer,cyclization,and relaxation,and the possible reaction path was revealed by the density functional theory(DFT)*** reaction conditions of photosensitizer type and addition,molar ratio of substrates,reaction temperature,and incident light intensity were optimized,with the target product yield achieving 65.5%.Moreover,the reaction dynamics of the reaction rate versus the light intensity are *** the hydrogenation-deoxygenation reaction,three fuels with a high density of 0.864-0.938 g·ml^(-1) and a low freezing point of<-55℃ are *** work provides a benign and effective approach to synthesize high-performance fuels.

关键词： High-energy-density fuel Transposed Patern-oeBüchi reaction Kinetics Bioenergy Photochemistry

A review of reservoir damage during hydraulic fracturing of deep and ultra-deep reservoirs

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Petroleum Science 2024年第1期21卷 384-409页

作者： Kun Zhang Xiong-Fei Liu Dao-Bing Wang Bo Zheng Tun-Hao Chen Qing Wang Hao Bai Er-Dong Yao Fu-Jian Zhou National Key Laboratory of Petroleum Resources and Engineering China University of Petroleum-BeijingBeijing102249China School of Mechanical Engineering Beijing Institute of Petrochemical TechnologyBeijing102617China Tuha Downhole Operation Company CNPC Xibu Drilling Engineering Company LimitedShanshan838200XinjiangChina

Deep and ultra-deep reservoirs have gradually become the primary focus of hydrocarbon exploration as a result of a series of significant discoveries in deep hydrocarbon exploration *** reservoirs present unique challenges due to their deep burial depth(4500-8882 m),low matrix permeability,complex crustal stress conditions,high temperature and pressure(HTHP,150-200℃,105-155 MPa),coupled with high salinity of formation ***,the costs associated with their exploitation and development are exceptionally *** deep and ultra-deep reservoirs,hydraulic fracturing is commonly used to achieve high and stable *** hydraulic fracturing,a substantial volume of fluid is injected into the ***,statistical analysis reveals that the flowback rate is typically less than 30%,leaving the majority of the fluid trapped within the ***,hydraulic fracturing in deep reservoirs not only enhances the reservoir permeability by creating artificial fractures but also damages reservoirs due to the fracturing fluids *** challenging“three-high”environment of a deep reservoir,characterized by high temperature,high pressure,and high salinity,exacerbates conventional forms of damage,including water sensitivity,retention of fracturing fluids,rock creep,and proppant *** addition,specific damage mechanisms come into play,such as fracturing fluid decomposition at elevated temperatures and proppant diagenetic reactions at HTHP ***,the foremost concern in deep oil and gas development lies in effectively assessing the damage inflicted on these reservoirs by hydraulic fracturing,comprehending the underlying mechanisms,and selecting appropriate ***'s noteworthy that the majority of existing studies on reservoir damage primarily focus on conventional reservoirs,with limited attention given to deep reservoirs and a lack of systematic *** light of this,our approach entails initially summarizin

关键词： Artificial fracture Deep and ultra-deep reservoir Fracture conductivity Fracturing fluid Hydraulic fracturing Reservoir damage