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Thermogravimetric characteristics of corn straw and bituminous coal copyrolysis based the ilmenite oxygen carriers

Chinese Journal of chemical engineering 2024年第4期68卷 8-15页

作者： Pengxing Yuan Xiude Hu Jingjing Ma Tuo Guo Qingjie Guo College of Chemical Engineering Qingdao University of Science&TechnologyQingdao 266042China State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering Ningxia UniversityYinchuan 750021China

Herein,the co-pyrolysis reaction characteristics of corn straw(CS)and bituminous coal in the presence of ilmenite oxygen carriers(OCs)are investigated via thermogravimetry coupled with mass *** results reveal that the participation of OCs weakens the devolatilization intensity of *** the CS blending ratio is<50%,the mixed fuel exhibits positive synergistic *** fitting results according to the Coats-Redfern integral method show that the solid-solid interaction between OCs and coke changes the reaction kinetics,enhancing the co-pyrolysis reactivity at the high-temperature zone(750-950C).The synergistic effect is most prominent at a 30%CS blending ratio,with copyrolysis activation energy in the range of 26.35-40.57 kJ·mol^(-1).

关键词： Oxygen carrier Co-pyrolysis Biomass Coal

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Oxygen vacancy-rich CoMoO4/Carbon nitride S-scheme heterojunction for boosted photocatalytic H_(2)production:Microstructure regulation and charge transfer mechanism

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Journal of Materials Science & technology 2024年第31期198卷 176-185页

作者： Jiani Qin Yanli Dong Xiaojuan Lai Bo Su Bao Pan Chuanyi Wang Sibo Wang School of Environmental Science and Engineering Shaanxi University of Science and TechnologyXi'an 710021China Key Laboratory of Chemical Additives for China National Light Industry School of Chemistry and Chemical EngineeringShaanxi University of Science and TechnologyXi'an 710021China State Key Laboratory of Photocatalysis on Energy and Environment College of ChemistryFuzhou UniversityFuzhou 350116China

Developing highly efficient S-scheme photocatalysts is a subject of immense interest for harnessing solar energy towards sustainable hydrogen ***,a novel S-scheme heterojunction of oxygen vacancy-rich CoMoO_(4)/CN(CMO/CN)photocatalyst was rationally constructed through loading CoMoO_(4)nanorods on carbon nitride(CN)nanosheets via a direct one-pot calcination *** CMO/CN S-scheme heterojunction exhibited enhanced surface area,fine CN dispersion,rich oxygen vacancies,and accelerated charge separation/transfer efficiency,which were conducive to improving photocatalytic H_(2)evolution *** note,the optimal 3%CMO/CN sample displayed the highest H_(2)production rate of 8.35 mmol g^(-1)h^(-1),which is 4.6 folds that of pristine *** situ irradiated X-ray photoelectron spectroscopy(XPS)and electron paramagnetic resonance(EPR)characterizations confirmed the S-scheme charge transfer path between CN and CMO,which greatly promoted spatial charge *** functional theory(DFT)calculations together with contact angle tests revealed the reduced activation energies for H_(2)O dissociation and enhanced hydrophilicity of the CMO/*** CMO/CN photocatalysts also presented high stability and fine *** work may provide insights into the combination of defect engineering and heterojunction designing for high-efficiency solar-to-chemical energy conversion.

关键词： S-scheme CoMoO_(4) Carbon nitride Oxygen vacancy Photocatalysis

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Tandem electrocatalysis for CO_(2) reduction to multi-carbons

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Science China Chemistry 2024年第11期67卷 3631-3651页

作者： Xindi Li Tianxiang Yan Yichen Meng Zhanpeng Liang Tianying Zhang Haoyuan Chi Ziting Fan Yifan Jin Haoran Zhang Sheng Zhang Key Laboratory for Green Chemical Technology of Ministry of Education Collaborative Innovation Centre of Chemical Science and EngineeringSchool of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China Haihe Laboratory of Sustainable Chemical Transformations Tianjin 300192China Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityFuzhou 350207China

The rising CO_(2) concentration in the atmosphere due to extensive use of fossil fuels has led to serious climate and environmental issues. One efficient solution is that CO_(2) capture from industrial emissions followed its conversion into value-added chemicals driven by renewable energies. CO_(2) electroreduction(CO_(2) RR) features a green and sustainable fashion towards effective CO_(2) conversion, but still suffers from low multi-carbon selectivity and yield. Considering the pivotal role of CO intermediate in C–C coupling to multi-carbon formation, tandem CO_(2) RR systems with separated CO generation and consumption components could facilitate the coupling between *CO-based intermediates to energy-intensive multi-carbons by manipulating CO diffusion and surface coverage. In this aspect, we comprehensively reviewed the design principles of tandem systems for CO_(2) electroreduction reaction. The chemistry behind the C–C coupling regarding to their distribution and diffusion was initially introduced, which was followed by achievements on tandem architectures, from catalysts, electrodes to systems. Future directions and perspectives on advanced tandem system designs for CO_(2) RR were discussed at the end. This review contributes to the understanding of structureperformance correlations in tandem catalysis and helps guide the effective collection of multi-carbons of high-yield and highselectivity.

关键词： electrocatalytic CO_(2)reduction tandem electrocatalysis design CO mass transfer model

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Coordination of distinctive pesticide adjuvants and atomization nozzles on droplet spectrum evolution for spatial drift reduction

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Chinese Journal of chemical engineering 2024年第2期66卷 250-262页

作者： Shidong Xue Jingkun Han Xi Xi Zhong Lan Rongfu Wen Xuehu Ma State Key Laboratory of Fine Chemicals Liaoning Key Laboratory of Clean Utilization of Chemical ResourcesInstitute of Chemical EngineeringSchool of Chemical EngineeringDalian University of TechnologyDalian 16024China School of Fashion and Textiles The Hong Kong Polytechnic UniversityHong Kong 999077China China Tianchen Engineering Corporation Tianjin 300400China School of Energy and Power Engineering Dalian University of TechnologyDalian 116024China

Pesticide adjuvants,as crop protection products,have been widely used to reduce drift loss and improve utilization efficiency by regulating droplet ***,the coordinated regulation mechanisms of adjuvants and nozzles on droplet spectrum remain ***,we established the relationship between droplet spectrum evolution and liquid atomization by investigating the typical characteristics of droplet diameter distribution near the *** on this,the regulation mechanisms of distinctive pesticide adjuvants on droplet spectrum were clarified,and the corresponding drift reduction performances were quantitively evaluated by wind tunnel *** shows that the droplet diameter firstly shifts to the smaller due to the liquid sheet breakup and then prefers to increase caused by droplet *** the surface tension of sprayed liquid facilitates the uniform liquid breakup and increasing the viscosity inhibits the liquid deformation,which prolong the atomization process and effectively improve the droplet *** a result,the drift losses of flat-fan and hollow cone nozzles are reduced by about 50%after adding organosilicon and vegetable oil *** contrast,the air induction nozzle shows a superior anti-drift ability,regardless of distinctive *** findings provide insights into rational adjuvant design and nozzle selection in the field application.

关键词： Pesticide drift Spray droplets Particle size distribution Spray atomization Transport processes Adjuvants

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π-conjugated chromophore functionalized high-nuclearity titanium-oxo clusters containing structural unit of anatase for photocatalytic selective oxidation of sulfides

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Rare Metals 2024年第4期43卷 1736-1746页

作者： Ling-Rong Liao Dong-Chun Zheng Pin-Xi Ou Qi-Xin Zhao Wei-Min Xuan Qi Zheng State Key Laboratory for Modification of Chemical Fibers and Polymer Materials&College of Materials Science and Engineering Donghua UniversityShanghai201620China State Key Laboratory for Modification of Chemical Fibers and Polymer Materials and College of Chemistry and Chemical Engineering Donghua UniversityShanghai 201620China

N-doping has significant influence in manipulating the properties of TiO_(2),and this has stimulated the development of N-donor-functionalized titanium-oxo clusters(TOCs)as molecular models to study the structure-property ***,the structural type and photoresponsive application are still limited for such TOCs,especially regarding the high-nuclearity TOCs that contain structure unit of TiO_(2)for ***,we showed the synthesis of a series of high-nuclearity TOCs 1-3 compounds usingπ-conjugated 1,10-phenanthroline(phen)as chromophore and N-donor functional *** 1 features cocrystal structure composed of one[Ti_(26)]~(2+)and half[Ti_(22)]~(2+),which renders it as the first cocrystallized TOC containing two positively charged species and phen-functionalized TOC showing the highest nuclearity up to 37 Ti *** adjusting the synthetic conditions,the individual{Ti_(22)}and{Ti_(26)}clusters can also be isolated as Compounds 2 and 3,*** core structure of{Ti_(22)}is mainly constructed from four lacunary{Ti_(4)}derived from pentagonal{Ti(Ti)_5}unit,while{Ti_(26)}is built from four complete{Ti(Ti)_5}***,a{Ti_8O_(14)}structure unit of anatase TiO_(2)can be identified in{Ti_(26)}.Based on the unique structural features and proper photophysical and photochemical properties of Compounds 1-3,they are applied for photocatalytic *** to the presence of anatase structure unit in{Ti_(26)}and the synergistic effect from{Ti_(22)}and{Ti_(26)},the catalytic performance presents in the order of Compound 1>Compound 3>Compound *** work provides excellent models to understand the structureproperty relationship from the perspective of cocrystallization and Ti-O binding model and will further promote the application of TOCs as functional catalysts for organic transformation.

关键词： Titanium-oxo cluster Molecular model of anatase TiO_(2) High nuclearity π-conjugated chromophore Photocatalytic sulfoxidation

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Recent progress in metal-organic frameworks(Part Ⅱ—material application)

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Science China Chemistry 2025年第5期68卷 1642-1702页

作者： Jiandong Pang Wentao Jiang Xue-Wen Zhang Hao-Long Zhou Yuxiu Sun Wei Gong Bin Wang Fuyin Ma Linwei He Long Chen Qiang Chen He-Qi Zheng Yuanjing Cui Wen-Jie Shi Chao Zhang Mei Wang Yue-Biao Zhang Jie-Peng Zhang Chongli Zhong Yong Cui Shuao Wang Jian-Rong Li Guodong Qian Tong-Bu Lu Huan Pang Xian-He Bu School of Materials Science and Engineering Nankai University School of Physical Science and Technology Shanghai Tech University MOE Key Laboratory of Bioinorganic and Synthetic Chemistry GBRCE for Functional Molecular EngineeringSchool of ChemistryIGCMESun Yat-sen University Department of Chemistry Shantou University School of Chemical Engineering and Technology Tiangong University School of Chemistry and Chemical Engineering Shanghai Jiao Tong University State Key Laboratory of Radiation Medicine and Protection School for Radiological and Interdisciplinary SciencesSoochow University College of Materials Science & Engineering Beijing University of Technology State Key Laboratory of Silicon and Advanced Semiconductor Materials Cyrus Tang Center for Sensor Materials and ApplicationsSchool of Materials Science & EngineeringZhejiang University Institute for New Energy Materials and Low Carbon Technologies School of Materials Science and EngineeringTianjin University of Technology School of Chemistry and Chemical Engineering Yangzhou University

As a class of functional crystalline porous materials, metal-organic frameworks(MOFs) gained rapid development in the past three decades and a large number of MOFs with ordered structures, high surface areas, and functionalized channels have been investigated. MOFs and MOF-derived/composite materials show great potential in many application fields. In this review, we discussed the main applications of MOFs and MOF-derived/composite materials in small molecule storage, separation, luminescence, sensing, multitype catalysis, and energy storage. In addition, challenges and problems in the future research of MOFs-related fields are also discussed.

关键词： metal-organic frameworks storage and separation sensing and detection multitype catalysis energy storage

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Tuning sodium wettability and pore tortuosity for superior sodium storage

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Rare Metals 2023年第12期42卷 4048-4059页

作者： Yao-Yao Xiao Yi-Hui Liu Bing-Bing Liu Zhen-Guo Qi You-Bin Zhang Fu-Sheng Liu Guo-Hui Qin State Key Laboratory Base for Eco-Chemical Engineering College of Chemical EngineeringQingdao University of Science and TechnologyQingdao 266042China Shandong Synergetic Innovation Center of Ecological and Chemical Engineering Qingdao 266042China

Abundant FeS2 with high theoretical capacity is one of the promising anode candidates in sodium-ion batteries(SlBs),however,the uneven sodium deposition due to the poor interface compatibility and sluggish reaction kinetics because of the high activation barrier still plague its practical ***,we synthesized the ordered porous carbon matrix wrapped FeS2 nanoparticles(FeS_2@OCN)with high sodium wettability and low pore tortuosity to economically enhance the interface compatibility as well as to lower the energy barrier in *** synergistic effects of low tortuosity pores and strong sodium wettability homogenize the Na+flux distribution,bring the electron dislocation via the enrichment of edgenitrogen(Pyridinic N and Pyrrolic N),thus achieving the dendrite-free sodium deposition and dramatically enhanced reaction *** from exceptional structural/compositional/electronic merits,the resultant anode is endowed with exceptional structure stability,achieving long-term cycling stability of 451.9 mAh·g^(-1)after 1000cycles at 1 A·g^(-1)with specific capacity retention of 92.9%.Attenuated electrode tortuosity and high sodium wettability can corporately improve the interface compatibility and attenuate the activation barrier of the FeS_2 host and beyond.

关键词： FeS_2 Wettability Sodium capture Low tortuosity Charge transport

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Revealing the anti-sintering phenomenon on silica-supported nickel catalysts during CO_(2)hydrogenation

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Journal of Environmental Sciences 2024年第6期140卷 270-278页

作者： Liuqingqing Yang Tiancheng Pu Feixiang Tian Yulian He Minghui Zhu State Key Laboratory of Chemical Engineering School of Chemical EngineeringEast China University of Science and TechnologyShanghai 200237China University of Michigan-Shanghai Jiao Tong University Joint Institute Shanghai Jiao Tong UniversityShanghai 200240China School of Chemistry and Chemical Engineering Shanghai Jiao Tong UniversityShanghai 200240China

The CO_(2)catalytic hydrogenation represents a promising approach for gas-phase CO_(2)utilization in a direct *** to its excellent hydrogenation ability,nickel has been widely studied and has shown good activities in CO_(2)hydrogenation reactions,in addition to its high availability and low ***,Ni-based catalysts are prone to sintering under elevated temperatures,leading to unstable catalytic *** the present study,various characterization techniques were employed to study the structural evolution of Ni/SiO_(2)during CO_(2)*** anti-sintering phenomenon is observed for both 9%Ni/SiO_(2)and 1%Ni/SiO_(2)during CO_(2)hydrogenation at 400℃.Results revealed that Ni species were re-dispersed into smaller-sized nanoparticles and formed Ni^(0)active *** interestingly,this anti-sintering phenomenon leads to distinct outcomes for two catalysts,with a gradual increase in both reactivity and CH_(4)selectivity for 9%Ni/SiO_(2)presumably due to the formation of abundant surface Ni°from redispersion,while an apparent decreasing trend of CH_(4)selectivity for 1%Ni/SiO_(2)sample,presumably due to the formation of ultra-small nanoparticles that diffuse and partially filled the mesoporous pores of the silica support over ***,the redispersion phenomenon was found relevant to the H_(2)gas in the reaction environment and enhanced as the H_(2)concentration *** finding is believed to provide in-depth insights into the structural evolution of Ni-based catalysts and product selectivity control in CO_(2)hydrogenation reactions.

关键词： Carbon dioxide utilization CO_(2)hydrogenation Nickel-based catalysts Anti-sintering Structural evolution

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Upcycling of polyethylene terephthalate to 1,4-cyclohexanedimethanol in water

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Science China Chemistry 2025年第5期68卷 2101-2109页

作者： Shuhui Fang Zhiwen Gao Xinrui Shi Min Zhang Wei Zhang Yue Liu State Key Laboratory of Petroleum Molecular & Process Engineering Shanghai Key Laboratory of Green Chemistry and Chemical ProcessesSchool of Chemistry and Molecular EngineeringEast China Normal University Engineering Center for Sustainable Carbon Science and Technology East China Normal University Institute of Eco-Chongming

The recycling of waste polyethylene terephthalate（PET）, an extensively used polymer as plastic and fiber materials, has become an urgent topic due to the rapid generation and accumulation of plastic waste into the environment. Current chemical recycling approaches to depolymerize and convert PET into 1,4-cyclohexanedimethanol（CHDM）, an important chemical in the production of advanced polyesters, predominantly use organic solvents, such as alcohols or dioxane. Herein, we developed an environmentally friendly and economically viable pathway for converting PET to CHDM using water as the solvent. In this process, PET is sequentially hydrolyzed in water, hydrogenated to 1,4-cyclohexane dicarboxylic acid（CHDA）, and then reduced to CHDM. The PET conversion rate is self-enhanced in aqueous medium via acid-catalyzed hydrolysis by the generated CHDA intermediate. A Pd-based catalyst（e.g., Pd/C） selectively hydrogenates the arene ring of the PET monomer, terephthalic acid intermediate, and a Ru-Sn/C bimetallic catalyst reduces its COOH to CH2OH group. At optimized reaction conditions, a complete conversion of PET and 80.1% yield of CHDM are obtained. Alternatively, this approach can also efficiently produce CHDA from PET, with a yield up to 86.4%.

关键词： polyethylene terephthalate (PET) 1,4-cyclohexanedimethanol (CHDM) hydrogenation hydrogenolysis

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Selective adsorption of liquid long-chainα-olefin/paraffin on Mg-MOF-74:Adsorption behavior and interaction mechanism

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Nano Research 2023年第1期16卷 1595-1605页

作者： Ruihan Yang Shafqat Ullah Xiao Chen Junxiang Ma Yuan Gao Yujun Wang Guangsheng Luo State Key Lab of Chemical Engineering Department of Chemical EngineeringTsinghua UniversityBeijing 100084China Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical EngineeringTsinghua UniversityBeijing 100084China Lu’an Chemical Group Co. Ltd.Changzhi 046299China

The liquid products of Fischer–Tropsch synthesis with a high content of linearα-olefins can act as valuable raw materials for increasing high added-valueα-olefin production if the challenging separation of long-chainα-olefin/paraffin is *** separation is an efficient alternative to energy-intensive ***,the selective adsorption behavior and interaction mechanism of liquidα-olefin/paraffin on Mg metal–organic framework(MOF)-74 were investigated using a combination of batch adsorption experiments and molecular simulation ***-MOF-74 exhibited 301 and 333 mg/g olefin adsorption capacities for C6 and C8 linearα-olefins in binary olefin/paraffin mixtures,respectively,and was still unsaturated at high olefin *** adsorption isotherms were analyzed and compared with the simulated results by configurational-bias grand canonical Monte Carlo(CB-GCMC)*** visualized adsorption sites by CB-GCMC simulation indicated that all adsorbates were arranged in hexagonal shapes and preferentially adsorbed by the vertex of the hexagon,where the metal node magnesium is *** adsorption energies were−1.456 and−0.378 eV for C8 linearα-olefin and paraffin,respectively,calculated by density functional theory simulation based on the visualized adsorption *** charge transfer was analyzed,and the contributions of different kinds of interactions to the overall adsorption energy were quantified by principle orbital interaction analysis to further reveal the difference in adsorption energy betweenα-olefin/paraffin and *** work also provides a general means to investigate the liquid adsorption performance and host–guest interactions in the adsorption or catalytic processes of nanoporous materials.

关键词： linearα-olefin metal-organic frameworks liquid-phase adsorption molecular simulations principle orbital interaction

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