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Chinese Chemical Letters 2021年第3期32卷 1127-1130页

作者： Jiyuan Liu xueqing gong Key Laboratory for Advanced Materials Centre for Computational Chemistry and Research Institute of Industrial CatalysisSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237China

CO oxidation at ceria surfaces has been studied for decades,and many efforts have been devoted to understanding the effect of surface reduction on the catalytic *** this work,we theoretically studied the CO oxidation on the clean and reduced CeO_(2)(111)surfaces using different surface cells to dete rmine the relationships between the reduction degrees and calculated reaction *** is found that the calculated barrier for the direct reaction between CO and surface lattice O drastically decreases with the increase of surface reduction *** electronic analysis,we found that the surface reduction can lead to the occurrence of localized electrons at the surface Ce,which affects the charge distribution at surface *** the result,the surface O becomes more negatively charged and therefore more active in reacting with *** work then suggests that the localized 4 f electron reservoir of Ce can act as the"pseudo-anion"at reduced CeO_(2) surfaces to activate surface lattice O for catalytic oxidative reactions.

关键词： CO oxidation CeO_(2)(111) Mars-van krevelen mechanism DFT+U Surface reduction

Genetic algorithm aided density functional theory simulations unravel the kinetic nature of Au(100) in catalytic CO oxidation

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Chinese Chemical Letters 2019年第6期30卷 1346-1350页

作者： Yi Fang xueqing gong Key Laboratory for Advanced Materials Centre for Computational Chemistry and Research Instiute of Industrial CatalysisSchool of Chemistry Molecular EngineeringEast China University of Science and Technology

Heterogeneous catalysis is of tremendous importance to modern industries. Exposed atoms of heterogeneous catalysts are heavily involved in surface processes such as the adsorption, activation, diffusion and reaction of substrate molecules. Surfaces of metal or metal oxide based catalysts are usually taken as hard templates that only undergo limited relaxation during catalytic reactions, especially in theoretical simulations. In this work, by using genetic algorithm (GA) aided density functional theory (DFT) calculations, we studied the surface processes involved in CO oxidation on the Au(100) surface. The use of GA greatly improves the capacity of DFT calculations in locating the potential energy surface (PES) of the surface reactions, and surprisingly, it has been found that the Au(100) surface can undergo drastic reconstruction under the influence of O adsorption and the adapted partially oxidized Au surface exhibits unique activities for subsequent adsorptions and reactions. This work depicts the kinetic nature of the Au (100) surface in its catalyzed reactions and also significantly expands our understanding of how surface atoms act in heterogeneous catalysis.

关键词： Gold catalysts Genetic algorithm Density functional theory Potential energy surface Surface reconstruction

A comparative DFT+U study of CO oxidation on Pd-and Zr-doped ceria

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Journal of Rare Earths 2023年第7期41卷 1042-1048,I0003页

作者： Lu Chen Xinping Wu xueqing gong Key Laboratory for Advanced Materials and Joint International Research Laboratory for Precision Chemistry and Molecular Engineering Feringa Nobel Prize Scientist Joint Research CenterFrontiers Science Center for Materiobiology and Dynamic ChemistryCentre for Computational Chemistry and Research Institute of Industrial CatalysisSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237China

Metal-doped ceria catalysts have been applied in many important catalytic *** this work,we performed density functional theory calculations corrected by on-site Coulomb interactions to study the Pd-and Zr-doped CeO_(2)(111) surfaces with the dopant at different *** formation of oxygen vacancies and CO oxidation were systematically calculated on the various doped *** find that both Pd and Zr doping can activate the surface lattice O and reduce the energy barriers of CO ***,the promotion effect of the Zr dopant is limited to its existence in the first surface layer,while for the Pd dopant,the surface activity can be greatly enhanced even it occurs far below the ***,CO_(2) can be generated directly on the Pd-doped surfaces through reaction between CO and surface O,while the surface intermediate CO_(2)^(δ-) may readily form and restrict the releasing of CO_(2) by further oxidation to carbonates on the Zr-doped *** analyses show that the doped Pd exists as Pd^(4+) and it has stronger electron affinity than other surface species during CO oxidation,contributing to the easy Pd^(4+) to Pd^(2+) transformation accompanied by direct CO_(2) formation at Pd-doped ceria.

关键词： CeO_(2) Metal doping CO oxidation Carbonate DFT+U Rare earths

FeOOH photo-deposited perylene linear polymer with accelerated charge separation for photocatalytic overall water splitting

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Science China Chemistry 2022年第1期65卷 170-181页

作者： Haonan Ye Zhiqiang Wang Ke Hu Wenjun Wu xueqing gong Jianli Hua Key Laboratory for Advanced Material Feringa Nobel Prize Scientist Joint Research CenterSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237China Key Laboratory for Advanced Materials Centre for Computational Chemistry and Research Institute of Industrial CatalysisSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237China Department of Chemistry Fudan UniversityShanghai 200433China

It is a challenge to develop single polymer-based photocatalyst for overall water splitting without adding sacrificial agents due to the insufficient driving force for charge separation and the lack of active sites of organic *** oxyhyroxides are widely acted as co-catalyst for photoelectrocatalysis oxygen evolution ***,we firstly report the peryleno[1,12-bcd]thiophene sulfone-based linear co-polymer PS-5 for photocatalytic overall water splitting by photo-depositing simple and low-cost cocatalyst FeOOH under the visible-light *** density functional theory(DFT)calculations and experimental results indicated clearly that the oxygen vacancies-richβ-FeOOH can effectively promote the separation of photo-generated excitons and provide active sites for photocatalytic oxygen evolution *** a result,the average H_(2)and O_(2)production rates of optimized PS-5/β-FeOOH-0.2M reach at~170 and~76.6μmol h^(-1)g^(-1),respectively,with a stoichiometric ratio at about 2:*** work provides a simple and low-cost method for the preparation of overall water splitting system based on polymer photocatalyst.

关键词： photocatalysis conjugated polymers FeOOH photo-deposited overall water splitting

Realization approach of Pd-only three-way catalysts with high catalytic performance and thermal stability

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Science China Chemistry 2015年第1期58卷 123-130页

作者： Yutao Ren Qun Shen Yun Guo Yanqin Wang Yanglong Guo xueqing gong Guanzhong Lu Key Laboratory for Advanced Materials and Research Institute of Industrial Catalysis East China University of Science and Technology

Pd-only three-way catalyst （TWC）, Pd supported on washcoating （the mixture of alumina and Ce-Zr solid solution）/cordierite, was prepared and its catalytic performance and the operation window （2-value） at 450 ℃ were evaluated with the simulated automotive exhaust feed gas. Surfactants such as Tween-80 and Span-20 were added in the process of preparing the catalyst in order to improve the thermal stability and catalytic performance of Pd-only TWC. The fresh and aged catalysts at 1000 ℃ for 4 h were characterized by low-temperature N2 adsorption, XRD, XPS, and H2-TPR techniques. The results show that the presence of surfactants in the synthesis slurry could influence the physicochemical properties of the final Pd-only TWC. The FTS catalyst prepared with the mixed surfactant of Tween-80 and Span-20 exhibited excellent three-way catalytic performance. After being aged at 1000℃ for 4 h, the catalytic performances of Pd-only TWCs slightly decreased, but the FTS catalyst still demonstrated higher catalytic performance and better thermal stability compared with the Pd-only catalysts prepared with single surfactant or without any surfactant. And the FTS catalyst has a wider 2 value （operation window） than other catalysts, even after being aged at 1000℃.

关键词： three-way catalyst Pd-only catalyst catalyst preparation mixed surfactants high thermal stability

Enhanced recycling performance of bimetallic Ir-Re/SiO_(2) catalyst by amberlyst-15 for glycerol hydrogenolysis

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Chinese Journal of Chemical Engineering 2022年第5期35卷 171-181页

作者： Xin Ren Li Leng Yueqiang Cao Jing Zhang Xuezhi Duan xueqing gong Jinghong Zhou Xinggui Zhou State Key Laboratory of Chemical Engineering East China University of Science and TechnologyShanghai 200237China Key Laboratory for Advanced Materials Centre for Computational Chemistry and Research Institute of Industrial CatalysisEast China University of Science and TechnologyShanghai 200237China

Recycling performance of heterogeneous catalysts is of crucial importance especially for a batch reaction *** this work,we demonstrate a strategy for enhancing recycling performance of Ir-Re/SiO_(2) catalyst synergized with amberlyst-15 in glycerol hydrogenolysis to produce 1,*** characterization results reveal that the Re sites in the Ir-Re/SiO_(2) catalyst undergo irreversible segregation and *** hinder the formation of active ReAOH species and thus contribute to a complete and irreversible ***,the introduction of amberlyst-15 into the reactant mixture can restrain the oxidation process of Re sites and favor the formation of ReAOH species,and thus significantly enhance the catalytic recycling *** results demonstrated here could guide the development of excellent bimetallic catalysts with the desirable recycling performances for the reaction.

关键词： Glycerol hydrogenolysis Ir-Re/SiO_(2)catalyst Deactivation mechanism Recycling performance Amberlyst-15 promoter

Efficient dye-sensitized solar cells based on concerted companion dyes:Systematic optimization of thiophene units in the organic dye components

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Chinese Chemical Letters 2022年第9期33卷 4313-4316页

作者： Jiaxin Luo Zhengli Xie Jiazhi Zou Xinyan Wu xueqing gong Chengjie Li Yongshu Xie Key Laboratory for Advanced Materials and Institute of Fine Chemicals Centre for Computational Chemistry and Research Institute of Industrial CatalysisSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237China

To develop efficient concerted companion(CC)dyes for fabricating high-performance DSSCs,three organic dyes XL1-XL3 have been designed by varying the position and number of theβ-hexylthiophene(HT)bridges,and these organic dye units are covalently linked with our previously reported porphyrin dye XW10 to construct the corresponding CC dyes *** the organic dyes,XL3 contains twoβ-hexylthiophene units at both the donor and acceptor parts and thus possesses stronger light-harvesting capability in the green light *** of the most complementary absorption between XL3 and XW10 as well as the excellent photovoltaic behavior of the individual XL3 dye,the corresponding CC dye XW76 affords the best PCE(10.78%)among all the CC *** coadsorption with CDCA,XW76 affords a highest PCE of 11.35%,which outperforms the previous cosensitization system of XW10+*** work provides an approach for developing efficient DSSCs based on CC dyes composed of an organic dye unit with suitableπspacers inserted at appropriate positions.

关键词： Dye sensitized solar cells Concerted companion dyes Porphyrin dyes Cosensitization

Methanol Dynamically Activated Room-Temperature Phosphorescence from a Twisted 4-Bromobiphenyl System

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CCS Chemistry 2020年第3期2卷 158-167页

作者： Zhiyi Yuan Jie Wang Lu Chen Lei Zou xueqing gong Xiang Ma Key Laboratory for Advanced Materials and Feringa Nobel Prize Scientist Joint Research Center School of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237

Crystal engineering is employed widely in developing metal-free room-temperature phosphorescence(RTP)materials,buttheweakresponsiveness inrigid stateand poor selectivity during crystallization limit the research of RTP materials with specific recognition ***,based on multicomponent crystallization and the deformation of phosphor,we have developed a galactose-functionalized polyhydric compound(BHB)with a twisted 4-bromobiphenyl structure,to realize methanol selectively activated“off–on”RTP *** molecules selectively formed solvate with BHB and rigidified the crystal structure by enriching intermolecular noncovalent ***,the distortion of the biphenyl group facilitated the intersystem crossing process effectively,alongside the heavy-atom effect from the bromo substitute,thereby,activating the RTP of *** our current research approach realizes RTPmaterials with selective recognition function by controlling multiple noncovalent interactions such as hydrogen and halogen bonding of molecular systems with structurally distorted phosphors.

关键词： room-temperature phosphorescence methanol identification structure deformation solvate

CeO_2(110)负载Au纳米颗粒催化CO+NO_x反应的DFT+U研究

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催化学报 2014年第8期35卷 1305-1317页

作者：张洁龚学庆卢冠忠华东理工大学结构可控先进功能材料及其制备教育部重点实验室计算化学中心工业催化研究所上海200237

通过在位库伦校正的密度泛函理论(DFT+U)方法计算,我们研究了CO和NOx分子在Au负载CeO2(110)表面的吸附.结果表明,CO在Au纳米颗粒的顶位有很强的吸附能,大约为1.2 eV,而NO在Au纳米颗粒上或者Au与CeO2载体界面处都是弱吸附.然而,当NOx在... 详细信息

通过在位库伦校正的密度泛函理论(DFT+U)方法计算,我们研究了CO和NOx分子在Au负载CeO2(110)表面的吸附.结果表明,CO在Au纳米颗粒的顶位有很强的吸附能,大约为1.2 eV,而NO在Au纳米颗粒上或者Au与CeO2载体界面处都是弱吸附.然而,当NOx在界面处形成N2O2二聚体之后,通过断裂末端的N–O键能够有效地被降解.纵观整个反应过程,第一步CO+N2O2的反应遵循了Langmuir-Hinshelwood机理,活化能只有0.4 eV,通过形成ONNOCO的中间物种最终产生N2O和CO2.不同的是,第二步消除N2O反应遵循了Eley-Rideal碰撞机理,需要相当高的能垒,约为1.8 eV.通过进一步分析表明,稀土Ce元素独特的电子特性能够使电子从Au上转移并且局域到载体表面的Ce阳离子上,并且有助于形成带负电的N2O2分子.而且Au纳米颗粒有很强的结构流动性,能够促进吸附的CO分子靠近界面处的N2O2并与之反应.

关键词：密度泛函理论三效催化剂二氧化铈金纳米颗粒一氧化碳氮氧化合物氧化还原反应电子局域

The synthesis of Co-doped SAPO-5 molecular sieve and its performance in the oxidation of cyclohexane with molecular oxygen

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Chinese Journal of Catalysis 2016年第2期37卷 273-280页

作者：校准詹望成郭耘郭杨龙龚学庆卢冠忠华东理工大学结构可控先进功能材料及其制备教育部重点实验室和工业催化研究所上海200237

Silicoaluminophosphate（SAPO） molecular sieves doped with cobalt（Co-SAPO-5） were synthesized hydrothermally with different concentrations of *** sample was characterized by X-ray diffraction,N2 adsorption-desorption,scanning electron microscopy,ultraviolet-visible spectroscopy,temperature-programmed desorption of NH3（NH3-TPD）,and infrared spectrascopy of adsorbed pyridine（Py-IR）.The results showed that Co was highly dispersed in the Co-SAPO-5 *** addition,a part of the Co content had been incorporated into the SAPO-5 framework,while the remainder existed on the surface as extra-framework *** surface areas of the Co-SAOP-5 samples were similar to the SAPO-5 ***,the pore volumes of the Co-SAOP-5 samples were lower than that of the SAOP-5 *** the concentration of Co increased,the pore volume gradually decreased because extra-framework cobalt oxide was present on the catalyst ***3-TPD and Py-IR results revealed that the amount of Br（？）nsted acid and the total amount of acid for the Co-SAPO-5 samples were higher than that for the SAPO-5 *** values were also higher for samples with higher Co *** catalytic activity of the Co-SAPO-5 samples was evaluated for the oxidation of cyclohexane with molecular *** Co was added to the SAPO-5 catalyst,the catalytic activity of the Co-SAPO-5 catalysts *** addition,the conversion of cyclohexane increased as the Co content in the Co-SAPO-5 catalysts ***,with a high conversion of cyclohexane（6.30%）,the total selectivity of cyclohexanone（K） and cyclohexanol（A） decreased *** K/A ratio ranged from 1.15 to *** effects of reaction conditions（i.e.,reaction temperature,reaction time,initial oxygen pressure,and the catalyst amount） on the performance of the Co-SAPO-5 catalysts have also been ***,the stability of the Co-SAPO-5 catalyst was explored and found to be good for the selective oxidation of cyclohexane by molecular oxygen.

关键词： SAPO-5 molecular sieve Cobalt Cyclohexane Selective oxidation Oxygen