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Nanoscale transition metal catalysts anchored on perovskite oxide enabling enhanced kinetics of lithium polysulfide redox in lithium-sulfur batteries

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Journal of Energy Chemistry 2023年第6期81卷 432-442,I0010页

作者： Wenshuo Hou Ruilong Li Zhenhua Wang Li Fang Zhe Bai Tan Wang Yu Bai Kening Sun Beijing Key Laboratory of Chemical Power Source and Green Catalysis School of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 100081China

To obtain high-performance lithium-sulfur(Li-S)batteries,it is necessary to rationally design electrocatalytic materials that can promote efficient sulfur electrochemical ***,the robust heterostructured material of nanoscale transition metal anchored on perovskite oxide was designed for efficient catalytic kinetics of the oxidation and reduction reactions of lithium polysulphide(Li PSs),and verified by density functional theory(DFT)calculations and experimental *** to the strong interaction of nanoscale transition metals with Li PSs through chemical coupling,heterostructured materials(STO@M)(M=Fe,Ni,Cu)exhibit excellent catalytic activity for redox reactions of Li *** bifunctional heterostructure material STO@Fe exhibits good rate performance and cycling stability as the cathode host,realizing a high-performance Li-S battery that can maintain stable cycling under rapid charge-discharge *** study presents a novel approach to designing electrocatalytic materials for redox reactions of Li PSs,which promotes the development of fast charge-discharge Li-S batteries.

关键词： Nanoscale transition metal Lithium polysulfide Catalytic activity Redox reaction Lithium-sulfur battery

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Exergy and exergoeconomic analyses for integration of aromatics separation with aromatics upgrading

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Frontiers of chemical Science and engineering 2023年第2期17卷 183-193页

作者： Dan Zhang Minbo Yang Xiao Feng Shaanxi Key Laboratory of Energy Chemical Process Intensification School of Chemical Engineering&TechnologyXi’an Jiaotong UniversityXi’an 710049China

Methanol to aromatics produces multiple products,resulting in a limited selectivity of *** upgrading is an effective way to produce more valuable xylene product,and different feed ratios generate discrepant product *** work integrates the aromatics separation with toluene disproportionation,transalkylation of toluene and trimethylbenzene,and isomerization of xylene and *** and exergoeconomic analyses are conducted to give insights in the splitting ratios of benzene,toluene and heavy aromatics for aromatics ***,a detailed simulation model is developed in Aspen ***,300 splitting ratio sets of benzene and toluene for conversion are studied to investigate the process *** results indicate that there are different preferences for the splitting ratios of benzene and toluene in terms of exergy and exergoeconomic *** process generates lower total exergy destruction when the splitting ratio of toluene varies between 0.07 and 0.18,and that of benzene fluctuates between 0.55 and ***,the process presents lower total product unit cost with the splitting ratio of toluene less than 0.18 and that of benzene fluctuating between 0.44 and ***,it is found that distillation is the biggest contributor to the total exergy destruction,accounting for 94.97%.

关键词： aromatics separation and upgrading variant splitting ratios total exergy destruction total product unit cost

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EDA-assisted synthesis of multifunctional snowflake-Cu_(2)S/CdZnS S-scheme heterojunction for improved the photocatalytic hydrogen evolution

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Journal of Materials Science & technology 2022年第26期121卷 28-39页

作者： Guorong Wang Yongkang Quan Kaicheng Yang Zhiliang Jin School of Chemistry and Chemical Engineering Ningxia Key Laboratory of Solar Chemical Conversion TechnologyKey Laboratory for Chemical Engineering and TechnologyState Ethnic Affairs CommissionNorth Minzu UniversityYinchuan 750021China

The charge separation efficiency is one of the main factors affecting the solar photocatalytic decomposition of water to produce *** a unique heterojunction can accelerate the separation and transfer of photo-generated charges,and effectively improve the photocatalytic efficiency,which is considered a potential ***,the 2%Cu_(2)S/CZS step-scheme(S-scheme)heterojunction based on morphology and electronic structure was successfully prepared via simple hydrothermal *** with the monomer Cu_(2)S and Cd Zn S,the hydrogen evolution rate of 2%Cu_(2)S/CZS samples is significantly *** particular,the 2%Cu_(2)S/CZS not only shows high hydrogen evolution rate of 5904μmol g^(-1)h^(-1)(3.19 times than original Cd Zn S),but also presents preferable cyclic *** to the characterization,we believe that the introduction of Cu_(2)S has the following three advantages:(i)The snowflake structure of Cu_(2)S reduces the agglomeration of granular Cd Zn S.(ii)The Cu_(2)S with narrow band gap broadens the light response range of the composite catalyst.(iii)The Cu_(2)S was introduced into Cd Zn S to form S-scheme heterojunction,which accelerated the separation and transfer of photo-generated *** work broadens the idea of designing efficient photocatalyst of hydrogen evolution.

关键词： S-scheme Heterojunction Multifunctional Snowflake-Cu_(2)S Photocatalyst

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Continuous amino-functionalized University of Oslo 66 membranes as efficacious polysulfide barriers for lithium−sulfur batteries

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Frontiers of chemical Science and engineering 2023年第2期17卷 194-205页

作者： Bowen Du Yuhong Luo Feichao Wu Guihua Liu Jingde Li Wei Xue Hebei Provincial Key Laboratory of Green Chemical Technology and High Efficient Energy Saving School of Chemical Engineering and TechnologyHebei University of TechnologyTianjin 300130China

The shuttle effect of soluble polysulfides is a serious problem impeding the development of lithium−sulfur ***,continuous amino-functionalized University of Oslo 66 membranes supported on carbon nanotube films are proposed as ion-permselective interlayers that overcome these issues and show outstanding suppression of the polysulfide shuttle *** proposed membrane material has appropriately sized pores,and can act as ionic sieves and serve as barriers to polysulfides transport while allowing the passage of lithium ions during electrochemical cycles,thereby validly preventing the shuttling of ***,a fast catalytic conversion of polysulfides is also achieved with the asdeveloped ***,lithium−sulfur batteries with this interlayer show a desirable initial capacity of 999.21 mAh·g^(-1)at 1 C and a durable cyclic stability with a decay rate of only 0.04%per cycle over 300 ***,a high area capacity of 4.82 mAh·cm^(-2)is also obtained even under increased sulfur loading(5.12 mg·cm^(-2))and a lean-electrolyte condition(E/S=4.8μL·mg^(-1)).

关键词： lithium−sulfur batteries aminofunctionalized University of Oslo 66 membrane polysulfide interlayer

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engineering of Ag@Pd/Al_(2)O_(3)with varied Pd-shell thickness:Dynamic evolution of ligand and strain effects on acetylene selective hydrogenation

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Chinese Journal of chemical engineering 2023年第12期64卷 139-148页

作者： Mingbo Yang Tianxing Yang Rui Ma Sha Li Yufei He Dianqing Li State Key Laboratory of Chemical Engineering Beijing University of Chemical TechnologyBeijing 100029China Department of Medicine and Chemical Engineering Lianyungang Technical CollegeLianyungang 222006China Chemistry and Chemical Engineering Guangdong Laboratory Shantou 515031China Quzhou Institute for Innovation in Resource Chemical Engineering Quzhou 324000China Beijing Engineering Center for Hierarchical Catalysts Beijing University of Chemical TechnologyBeijing 100029China

Bimetallic nanoparticles exhibit a synergistic effect that critically depends on their surface composition,but such promotion mechanisms become vague with varying surface ***,alumina supported Ag@Pd core–shell and PdAg alloy structure with controlled size and surface compositions were prepared to demonstrate synergetic mechanisms,particularly,ligand and strain effects on activity and ethylene selectivity for acetylene *** performance evaluation indicates that Ag@Pd catalysts with well-controlled Pd-shell thickness can effectively lower apparent activation energy and improve ethylene *** activity increases from 0.019 to 0.062 s^(-1) with decreasing Pd-shell thickness under mild conditions,which is 3–6 times higher than their alloyed and monometallic *** characterizations and density functional theory are conducted to reveal such shell-thickness-dependent *** ligand effect arising from Ag alloying in the interface of Ag@Pd2ML observes the strongest binding of acetylene,but it diminished sharply and the strain effect gets more prevailing with increasing shell *** competition of ethylene desorption and deephydrogenation were also investigated to understand the selectivity governing factors,and the selectivity descriptor(0.5BE(C_(2)H_(4))–BE(H))was built to match the contribution of ligand and strain effect on the different surfaces of Pd-Ag bimetallic *** exploration of synergetic mechanisms among bimetallic NPs with varied structure and surface compositions in this work can help us to deepen the understanding catalyst structure–activity relationship and provide a feasible way to optimize the overall catalytic performance.

关键词： Catalyst Hydrogenation Nanostructure Shell-thickness-dependent performance Ligand and strain effect

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Synthesis of tetrahedrally coordinated CoO for higher alcohol synthesis directly from syngas

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Frontiers of chemical Science and engineering 2024年第8期18卷 99-109页

作者： Zhuoshi Li Han Yang Xiaofeng Pei Jiahui Li Jing Lv Shouying Huang Yue Wang Xinbin Ma Key Laboratory for Green Chemical Technology of Ministry of Education Collaborative Innovation Center of Chemical Science and EngineeringSchool of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityBinhai New CityFuzhou 350207China Haihe Laboratory of Sustainable Chemical Transformations Tianjin 300192China

Higher alcohol synthesis directly from syngas is highly desirable as one of the efficient non-petroleum energy conversion ***^(0)–CoO catalysts showed great potential for this reaction,but the alcohol selectivity still needs to be improved and the crystal structure effect of Co^(0)on catalytic behaviors lacks ***,a series of tetrahedrally coordinated Co^(0)polymorphs were prepared by a thermal decomposition method,which consisted of wurtzite CoO and zinc blende CoO with varied *** diluting with SiO_(2),the catalyst showed excellent performance for higher alcohol synthesis with ROH selectivity of 45.8%and higher alcohol distribution of 84.1 wt%under the CO conversion of 38.0%.With increasing the content of wurtzite CoO,the Co^(0)/Co^(2+)ratio gradually increased in the spent catalysts,while the proportion of highly active hexagonal close packed cobalt in Co^(0)decreased,leading to first decreased then increased CO ***,the higher content of zinc blende CoO in fresh catalyst facilitated the retention of more Co^(2+)sites in spent catalysts,promoting the ROH selectivity but slightly decreasing the distribution of higher *** catalyst with 40%wurtzite CoO obtained the optimal performance with a space time yield toward higher alcohols of 7.9 mmol·gcat^(-1)·h^(-1).

关键词： higher alcohol synthesis CO hydrogenation wurtzite CoO zinc blende CoO hexagonal-closest-packed Co

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Built-in electric field intensified by photothermoelectric effect drives charge separation over Z-scheme 3D/2D In_(2)Se_(3)/PCN heterojunction for high-efficiency photocatalytic CO_(2) reduction

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Journal of Materials Science & technology 2024年第12期179卷 251-261页

作者： Hongjun Dong Lei Tong Pingfan Zhang Daqiang Zhu Jizhou Jiang Chunmei Li Institute of Green Chemistry and Chemical Technology School of Chemistry and Chemical EngineeringJiangsu UniversityZhenjiang 212013China School of Environmental Ecology and Biological Engineering Key Laboratory of Green Chemical Engineering Process of Ministry of EducationEngineering Research Center of Phosphorus Resources Development and Utilization of Ministry of EducationNovel Catalytic Materials of Hubei Engineering Research CenterWuhan Institute of TechnologyWuhan 430205China

It is a challenging issue to further drive charge separation through the oriented design of Z-scheme het-erojunction in the exploitation of cost-effective photocatalytic *** this contribution,the unique Z-scheme 3D/2D In_(2)Se_(3)/PCN heterojunction is developed through implanting In_(2)Se_(3) microspheres on PCN nanosheets using an in situ growth technique,which acquires the effective CO generation activity from photocatalytic CO_(2) reduction(CO_(2)R).The CO yield of 4 h in the CO_(2)R reaction over the optimal In_(2)Se_(3)/PCN-15 sample reaches up to 11.40 and 2.41 times higher than that of individual PCN and In_(2)Se_(3),*** greatly enhanced photocatalytic performance is primarily the improvement of photo-generated carrier separation *** be more specific,the formed built-in electric field is signifi-cantly intensified by producing the temperature difference potential between In_(2)Se_(3) and PCN owing to the photothermoelectric effect of In_(2)Se_(3),which actuates the high-efficiency separation of photogenerated charge carriers along the Z-scheme transfer path in the In_(2)Se_(3)/PCN *** effective strat-egy of enhancing the built-in electric field to drive photogenerated charge separation proposed in this work opens up an innovative avenue to design Z-scheme heterojunction applied to high-efficiency pho-tocatalytic reactions,such as hydrogen generation from water splitting,CO_(2)R,and degradation of organic pollutants.

关键词： In_(2)Se_(3)/PCN Z-scheme heterojunction Photocatalytic CO_(2) reduction Enhanced built-in electric field Photothermoelectric effect

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Facile Synthesis of Polycarbonate Diol via Copolymerization of CO_(2) and Cyclohexene Oxide Catalysed by a Combination of One-Component Phosphonium Borane Lewis Pair and Water

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Chinese Journal of Polymer Science 2023年第5期41卷 735-744,I0009页

作者： Xiao-Wu Wang Ji-Wen Hui Yu-Tao Li Yan-Ru Gu Zhi-Bo Li State Key Laboratory Base of Eco-Chemical Engineering/College of Chemical Engineering Qingdao University of Science and TechnologyQingdao 266042China Key Laboratory of Biobased Polymer Materials Shandong Provincial Education Department/School of Polymer Science and EngineeringQingdao University of Science and TechnologyQingdao 266042China

Well-defined polycarbonate diol was successfully synthesized through a strategy using a combination of organocatalyst and *** strategy was less developed in organocatalyzed polymerization and frequently regarded as side ***,one-component phosphonium borane Lewis pairs PB1-PB8 were successfully applied in the copolymerization of CO_(2) and cyclohexene oxide(CHO)to generate poly(CHO-alt-CO_(2))carbonate(PCHC).Parameters of linker length and counter anion effects on the catalyst activity were *** was found that Lewis pair PB3 served as a dual initiator and catalyst in the copolymerization of CHO and CO_(2) with or without the presence of *** contrast,Lewis pair PB8 can serve as a true catalyst for the preparation of well-definedα,ω-hydroxyl PCHC *** was achieved by introducing a labile CF3COO group as counter anion through anion exchange reaction while water molecules acted as chain transfer *** function of trifluoroacetate group in the polymerization process was investigated in detail and possible mechanism was *** changing the amount of water and catalyst loading,PCHC diols with varied molecular weight(1.5 kg/mol to 7.5 kg/mol),low dispersities(D<1.2)and carbonate content(>99%)could be easily *** low molecular weight PCHC diol was used as a bifunctional macroinitiator for the ring-opening polymerization of L-lactide(LLA)to afford ABA triblock copolymer in one-pot synthesis.

关键词： Polycarbonate Phosphonium borane Lewis pair CO_(2)utilization Organocatalysis Ring-opening polymerization

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A Ruddlesden-Popper oxide as a carbon dioxide tolerant cathode for solid oxide fuel cells that operate at intermediate temperatures

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Chinese Journal of chemical engineering 2023年第4期56卷 25-32页

作者： Shujun Peng Song Lei Sisi Wen Jian Xue Haihui Wang School of Chemistry&Chemical Engineering Jinggangshan UniversityJi'an 343009China School of Chemistry&Chemical Engineering Guangdong Provincial Key Lab of Green Chemical Product TechnologySouth China University of TechnologyGuangzhou 510640China Beijing Key Laboratory of Membrane Materials and Engineering Department of Chemical EngineeringTsinghua UniversityBeijing 100084China

Solid oxide fuel cells(SOFCs) that operate at intermediate temperatures of 600 to 800℃ have recently received increased attention due to their improved durability, more rapid startup and shutdown, better sealing and lower cost than their counterparts operate at high temperatures. Nevertheless, intermediatetemperature SOFCs(IT-SOFCs) with popular perovskite cathodes contain alkaline-earth elements, which are prone to reaction with carbon dioxide(CO_(2)), even when the CO_(2) content is comparatively low. In this work, an alkaline-earth metal-free Ruddlesden-Popper oxide, Nd_(1.8)La_(0.2)Ni_(0.74)Cu_(0.21)Ga_(0.05)O_(4+δ)(NLNCG), is developed for IT-SOFC cathodes. The cell is based on an electrolyte with 8%(mol) Y_(2)O_(3)-stabilized Zr O_(2)(8YSZ). The NLNCG cathode exhibits an excellent CO_(2) tolerance, as proven by thermogravimetry analysis,in situ X-ray diffraction, I-V-P test, and electrochemical impedance spectroscopy(EIS), and stability measurements. The anode-supported single-cell Ni O-YSZ|YSZ|NLNCG outputs a peak power density of 0.522 W·cm^(-2) at 800℃. These findings suggest that NLNCG could be a highly suitable cathode material with CO_(2) tolerance for IT-SOFCs.

关键词： Fuel cell Hydrogen Kinetics Catalyst CO_(2)tolerance

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Synthesis and Properties of Heat-resistant Polyimides Films Containing Crosslinkable Group-tetrafluorostyrene

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Chinese Journal of Polymer Science 2025年第5期43卷 863-874页

作者： Tian-Yong Zhang Jia-Ning Yu Sui-Sui Wang Ya-Mei Chai Shuang Jiang Hong-Li An Ruo-Xi Sun Bin Li Tianjin Key Laboratory of Applied Catalysis Science and Technology School of Chemical Engineering and TechnologyTianjin UniversityTianjin300354China Collaborative Innovation Center of Chemical Science and Engineering(Tianjin) Tianjin300072China Tianjin Engineering Research Center of Functional Fine Chemicals Tianjin300354China

Polyimide(PI)is widely used in high-tech fields such as microelectronics,aerospace,and national defense because of its excellent optical properties,high-and low-temperature resistance,and good dimensional *** achieve the desired properties of PI,the monomers 2,6-diaminopyrimidin-4-ol(DAPD)and 6-(2,3,5,6-tetrafluoro-4-vinylphenoxy)pyrimidin-2,4-diamine(DAFPD),which contains crosslinkable functional groups,were designed and synthesized successfully and copolymerized with 4,4'-oxydianiline(ODA)and 4,4-hexafluoroisopropylphthalic anhydride(6FDA).The prepared PI film(PI-3),with rigid backbones and loose packing had excellent heat resistance(Td5%=489℃)and optical properties(T450=82%).Furthermore,a crosslinked PI film(c-PI-3)with more heat-resistant(Td5%=524℃)and better mechanical properties(σ=125.46MPa),can be obtained through thermal crosslinking of *** addition,the changes in the properties caused by the proportion of DAFPD added during copolymerization are discussed *** study provides a promising candidate for heat-resistant PI materials.

关键词： Polyimide film Copolymerization Thermal crosslinking Heat resistance

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