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Reverse modulation of defect density of Ce-MOF-808 by solventassisted ligand exchange for dicyclopentadiene hydrogenation

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Science China Chemistry 2025年第06期 2744-2756页

作者： Danfeng Zhao Fajie Hu Rushuo Li Xinmeng Xu Zhaokun Wang Zuoshuai Xi Jun Tong Xiubing Huang Ge Wang Advanced Innovation Center for Materials Genome Engineering Beijing Key Laboratory of Function Materials for Molecule & Structure Construction School of Materials Science and Engineering University of Science and Technology Beijing

Defect engineering is a pivotal strategy for tailoring the electronic structure and physicochemical properties of catalysts, yet the straightforward manipulation of defect density in porous materials presents a current challenge. In this work, we achieved precise control over the coordination unsaturated site（CUS） content and pore architecture of Ce-MOF-808 by employing 2-fluorobenzoic acid（2-FBA） as a modifier. Leveraging the p Kadisparities among three ligands（1,3,5-tricarboxylic benzoic acid,formic acid, and 2-FBA）, we preserved the spn topology of Ce-MOF within an aqueous system, while realizing partial substitution of the auxiliary ligands and saturation of the CUS. The amount of 2-FBA was negatively correlated with the number of ligand defects, and the consequent decrease in Ce3+content and the increase in the number of ligand linkages also induced crystal structure transformation. The modulation of the defect structure was correlated with the catalytic performance of dicyclopentadiene（DCPD） hydrogenation reaction, in which Ce-MMF0.15, constructed by the modulation of 0.15 mol amount of 2-fluorobenzoic acid, exhibited an optimal ligand defect density and micro-mesoporous structure, enabling almost complete conversion of DCPD at 100 ℃ and 2 MPa. This article also elucidates the correlation between the regulation of defect density and the accessibility of frustrated Lewis pair（FLP） active sites, guiding the application of novel porous intrinsic FLP materials in hydrogenation catalysis.

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Magnetically-responsive phase change thermal storage materials:Mechanisms,advances,and beyond

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Journal of Energy Chemistry 2025年第2期101卷 485-510,I0010页

作者： Yan Gao Yang Li Jinjie Lin Panpan Liu Xiao Chen Ge Wang Beijing Advanced Innovation Center for Materials Genome Engineering Beijing Key Laboratory of Function Materials for Molecule&Structure ConstructionSchool of Materials Science and EngineeringUniversity of Science and Technology BeijingBeijing 100083China School of Physics and Astronomy Beijing Normal UniversityBeijing 100875China Shunde Graduate School University of Science and Technology BeijingFoshan 528399GuangdongChina

Rapid advances in thermal management technology and the increasing need for multi-energy conversion have placed stringent energy efficiency requirements on next-generation shape-stable composite phase change materials(PCMs).Magnetically-responsive phase change thermal storage materials are considered an emerging concept for energy storage systems,enabling PCMs to perform unprecedented functions(such as green energy utilization,magnetic thermotherapy,drug release,etc.).The combination of multifunctional magnetic nanomaterials and PCMs is a milestone in the creation of advanced multifunctional composite ***,a timely and comprehensive review of composite PCMs based on magnetic nanoparticle modification is still ***,we furnish an exhaustive exposition elucidating the cutting-edge advancements in magnetically responsive composite *** delve deeply into the multifarious roles assumed by distinct nanoparticles within composite PCMs of varying dimensions,meticulously scrutinizing the intricate interplay between their architectures and thermophysical ***,we prognosticate future research trajectories,delineate alternative stratagems,and illuminate prospective *** review is intended to stimulate broader academic interest in interdisciplinary fields and provide valuable insights into the development of next-generation magnetically-responsive composite PCMs.

关键词： Phase change materials Magnetic-thermal conversion Magnetic nanoparticles Thermal energy storage Response mechanism

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Recent advances in metal-loaded MOFs photocatalysts:From single atom,cluster to nanoparticle

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Chinese Chemical Letters 2025年第1期36卷 68-79页

作者： Shenglan Zhou Haijian Li Hongyi Gao Ang Li Tian Li Shanshan Cheng Jingjing Wang Jitti Kasemchainan Jianhua Yi Fengqi Zhao Wengang Qu Advanced Innovation Center for Materials Genome Engineering Beijing Key Laboratory of Function Materials for Molecule&Structure ConstructionSchool of Materials Science and EngineeringUniversity of Science and Technology BeijingBeijing 100083China National Key Laboratory of Energetic Materials Xi’an Modern Chemistry Research InstituteXi’an 710065China Shunde Innovation School University of Science and Technology BeijingShunde 528399China School of Materials Science and Engineering Suzhou University of Science and TechnologySuzhou 215009China Department of Chemical Technology Chulalongkorn UniversityBangkok 10330Thailand

Photocatalysis is widely regarded as a highly promising sustainable technique for addressing the challenges posed by environmental pollution and energy *** recent years,metal-loaded MOFs has become a rising star within the domain of photocatalysis due to its high specific surface area and porosity,adjustable structure,diverse and abundant catalytic components,which has exhibited excellent photocatalytic activity and exhibit great potential in a range of *** this paper,the principles for evaluating the photocatalytic performance of MOFs-based materials were firstly introduced,and some typical examples were also listed *** with this,particular emphasis is paid to the main factors affecting the photocatalytic performance of metal-loaded *** the synthesis and design strategies of MOFs loaded metal entities of varying sizes(single atoms,nanoclusters,and nanoparticles),and their applications in photocatalytic CO_(2)reduction,hydrogen production,photooxidation and photocatalytic hydrogenation were summarized and ***,the opportunities and challenges faced in this kind of MOFs-based composites were analyzed from different *** report is expected to help researchers design and develop high-performance MOFs-based photocatalytic materials.

关键词： Metal-loaded MOFs Photocatalysis Single atom catalysts Nanoclusters Nanoparticles

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Insights into structure-Activity Relationships between Y Zeolites and their n-C_(10)Hydrocracking Performances via Machine Learning Approaches

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Chinese Journal of Catalysis 2025年第4期71卷 187-196页

作者： Qianli Ma Hong Nie Ping Yang Jianqiang Liu Hongyi Gao Wei Wang Songtao Dong SINOPEC Research Institute of Petroleum Processing Co. Ltd.Beijing100083China Beijing Advanced Innovation Center for Materials Genome Engineering Beijing Key Laboratory of Function Materials for Molecule&Structure ConstructionSchool of Materials Science and EngineeringUniversity of Science and Technology BeijingBeijing 100083China

Hydrocracking technology represents a crucial position in the conversion of heavy oil and the transformation development from oil refining to the chemical *** properties of catalysts are one of the key factors in the hydrocracking *** the main acidic component of hydrocracking catalyst,the influence of zeolite properties on the reaction performance has been the focus of *** this study,a series of NiMo/Al_(2)O_(3)-Y catalysts were prepared using different Y zeolites as acidic components,and their performances in the hydrocracking of n-C_(10)were also *** structure-activity relationship between Y zeolite and the cracking performance of n-C_(10)was investigated with machine ***,a database of the physical and chemical properties of Y zeolite and their performance was established,and the correlation analysis was also *** such as the cell constant,acid content,acid strength,B/L ratio,mesopore volume,micropore volume of Y zeolite,and the reaction temperature were selected as independent *** conversion of n-C_(10)and the ratios of products C_(3)/C_(7)and i-C_(4)/n-C_(4)were selected as dependent variables.A model was established by the random forest algorithm and a new zeolite was predicted based on *** results of model prediction were in good agreement with the experimental *** R^(2)of the n-C_(10)conversion,C_(3)/C_(7)ratio,and i-C_(4)/n-C_(4)ratio were 0.9866,0.9845,and 0.9922,and the minimum root mean square error values were 0.0163,0.101,and 0.0211,*** results can provide reference for the development of high performance hydrocracking catalyst and technology.

关键词： Hydrocracking Machine learning Y zeolite n-Decane Acid Pore structure

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Multi-descriptors guided constructing the microenvironment of frustrated Lewis pair bi-active sites in functionalized MOFs toward Sabatier optimal for catalytic hydrogenation

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Journal of Catalysis 2025年 448卷

作者： Wang, Linmeng Feng, Shihao Gao, Hongyi Lu, Yunfeng Wang, Jingjing Wang, Ge Beijing Advanced Innovation Center for Materials Genome Engineering Beijing Key Laboratory of Function Materials for Molecule & Structure Construction School of Materials Science and Engineering University of Science and Technology Beijing Beijing100083 China Shunde Innovation School University of Science and Technology Beijing Shunde528399 China Department of Chemical and Biomolecular Engineering University of California Los AngelesCA90095 United States

Precise design and regulation of active site accessibility and chemical properties within metal–organic frameworks (MOFs) are crucial for enhancing catalytic performance, yet pose significant challenges. This study presents a design strategy for functionalized MOF-808 catalysts featuring frustrated Lewis pair (FLP) bi-active sites for catalytic hydrogenation. More specifically, we modulated the microenvironment of Lewis acid-base sites (LA-LB) by 4 categories of monocarboxylic acid ligands (i.e., the 6-substituted BR2 piperidine-2-carboxylic acid (FLP1-R), 1-substituted BR2 pyrazole-2-carboxylic acid (FLP2-R), 5-substituted BR2 pyrrolidine-2-carboxylic acid (FLP3-R) and 6-substituted BR2 pyridine-2-carboxylic acid (FLP4-R)) exchange, in which the LA coordinated the substituent group (−R) is −H, –OH, –NH2, –CH3, −Br, −Cl, −F, –NO2, −CF3, or –CN. Utilizing density functional theory (DFT), it elucidates the electronic-level regulation mechanisms affecting catalytic performance. We establish screening principles for 40 functionalized MOFs, revealing linear relationships between the geometric and electronic structures of the active moiety (neutral FLP-R) and both adsorption energy and Gibbs free energy barriers. Multi-descriptors, the dihedral angle between LA, LB and the critical points (c1 and c2) of electron localization function (ELF) upon dual active sites (φc1-LB-LA-c2), the distance of LA and LB (DLA&LB) and local chemical potential (μL) of FLP-R were firstly proposed to identify candidates favoring dissociative H2 adsorption over chemisorbed dicyclopentadiene (DCPD), thereby mitigating bi-active site due to strongly bound. Furthermore, the intrinsic descriptor |ΕpB|+|ΕpN| derived by the p band center of B atom (LA) and N atom (LB) yield an inverted volcano-shaped curve, with FLP3-CH3, FLP4-F, FLP4-CH3, and FLP4-OH functionalized MOF-808 positioned at the optimal point, balancing H2 dissociation and the hydrogenation of 8,9-dihydrodicyclopentadiene (8,9-DHDCPD). O

关键词： Dihedral angle

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Room-temperature synthesis of Co（OH）2/Mo2TiC2Tx hetero-nanosheets with interfacial coupling for enhanced oxygen evolution reaction

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Chinese Chemical Letters 2025年第04期 541-545页

作者： Lu Dai Yuxin Ren Shuang Li Meidi Wang Chentao Hu Ya-Pan Wu Guangtong Hai Dong-Sheng Li College of Materials and Chemical Engineering Key Laboratory of Inorganic Nonmetallic Crystalline and Energy Conversion Materials China Three Gorges University Hubei Three Gorges Laboratory Beijing Advanced Innovation Center for Materials Genome Engineering Beijing Key Laboratory of Function Materials for Molecule & Structure ConstructionSchool of Materials Science and Engineering University of Science and Technology Beijing

Constructing high-performance electrocatalysts for oxygen evolution reaction（OER） using a simple and economical strategy is considerably meaningful yet still challenging. Herein, Co（OH）2/Mo2Ti C2Tx（where Txrepresents the surface functional groups,-O,-OH and-F） hetero-nanosheets were facilely prepared by the in situ topochemical transformation at room temperature towards efficient OER. The integrity of Co（OH）2nanosheets and Mo2Ti C2Txnanosheets affords interfacial coupling to optimize the electronic structures of Co and Mo ions, which endows the high electron transfer efficiency and rapid reaction kinetics. As a result, the Co（OH）2/Mo2Ti C2Txhetero-nanosheets exhibit excellent OER performances with low overpotentials of 283 m V on glass-carbon electrode, and 227 m V on nickel foam at 10 m A/cm2. Furthermore, the decent anti-alkali ability underpins superior operational stability exceeding 100 h, demonstrating grand potential in practical applications. This work provides a new insight for the synthesis of efficient and cost-effective two-dimensional（2D） material-based electrocatalysts.

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Lanthanum-Mediated Enhancement of Low Temperature Hydrogenation Activity and Stability in Nickel Catalyst Supported by Mofs

SSRN

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SSRN 2025年

作者： Gao, Hongyi Liu, Zhiyuan Gao, Yan Wang, Changan Zhang, Yuanjie Yang, Ping Liu, Siqi Chen, Juan Liu, Zhimeng Wang, Jingjing Xu, Xinmeng Wang, Ge Beijing Advanced Innovation Center for Materials Genome Engineering Beijing Key Laboratory of Function Materials for Molecule & Structure Construction School of Materials Science and Engineering University of Science and Technology Beijing Beijing100083 China Shunde Innovation School University of Science and Technology Beijing Shunde528399 China Sinopec Research Institute of Petroleum Processing Co. Ltd SINOPEC Beijing100083 China

The development of low-cost, highly efficient, and durable non-noble metal catalysts for hydrogenation reactions has long posed a significant challenge in the field of catalysis. In this study, we present a novel non-noble metal catalyst, Ni/La NPs@UD, which consists of ultra-small nickel nanoparticles (NPs) modified with lanthanum (La) species and anchored on defective UiO-66 supports, specifically designed for the hydrogenation of dicyclopentadiene (DCPD). The incorporation of La not only enhances the electronic properties of the Ni centers but also facilitates effective electron transfer, promoting the formation of low-coordination, electron-rich Ni active sites that significantly improve hydrogen activation efficiency. Remarkably, at a mild temperature of 70 °C, Ni/La NPs@UD achieved 100% conversion of DCPD with a 99.9% selectivity for THDCPD, rivaling that of noble metal catalysts. Furthermore, the La species not only prevents the agglomeration of Ni NPs through a fencing effect but also mitigates the deposition of inert coke by increasing the density of medium strong basic sites. This dual action significantly prolongs the catalyst's lifespan, as evidenced by its sustained catalytic activity over 10 consecutive cycles. This findings underscore the potential of non-precious metal MOFs-based catalysts in achieving efficient hydrogenation under mild conditions, paving the way for their future application in sustainable chemical processes. © 2025, The Authors. All rights reserved.

关键词： Coke

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Constructing frustrated Lewis pairs on porous Ce-based metal-organic frameworks with improved dicyclopentadiene hydrogenation activity

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Chinese Chemical Letters 2025年第7期36卷

作者： Danfeng Zhao Jing Lin Rushuo Li Liang Chu Zhaokun Wang Xiubing Huang Ge Wang Advanced Innovation Center for Materials Genome Engineering Beijing Key Laboratory of Function Materials for Molecule & Structure Construction School of Materials Science and Engineering University of Science and Technology Beijing Beijing 100083 China

The construction of frustrated Lewis acid-base pairs (FLPs) in porous systems is very important for the field of industrial hydrogenation catalysis, but there is still a great challenge. Based on the Ce 3+ /Ce 4+ redox pairs and abundant defects in porous Ce-based metal-organic frameworks (Ce-MOFs), FLP sites consisting of ligand-defective Ce sites (Lewis acid, LA) and neighboring terminal O sites (Lewis base, LB) were constructed in situ by a simple vacuum thermal activation method in lamellar Ce-UiO-66-F. Defects/oxygen vacancies in the Ce-MOFs structure result in the difference in the electron cloud density between Ce and O, which is suitable for H H hetero-cleavage and H-transfer in the dicyclopentadiene (DCPD) hydrogenation process. Particularly, Ce-UiO-66-F-200 achieved 96.9 % conversion of DCPD and 97.8 % selectivity of 8,9-dihydrodicyclopentadiene (8,9-DHDCPD) at 100 °C under 2 MPa H2 for 10 h, which is 9.4 times higher than 10.2 % conversion of DCPD over the unactivated Ce-UiO-66-F. This research promotes the understanding of solid MOFs-based porous FLPs for H 2 activation, and encourages the in-depth investigation of surface solid FLPs to the whole material FLPs.

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Laminar-confined Co 9 S 8 quantum dots within layered hydroxide electrocatalyst for alkaline overall water splitting

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Journal of Alloys and Compounds 2025年 1031卷

作者： Zhaokun Wang Liang Chu Shibing Ren Mu Yang Ge Wang Beijing Advanced Innovation Center for Materials Genome Engineering Beijing Key Laboratory of Function Materials for Molecule & Structure Construction School of Materials Science and Engineering University of Science and Technology Beijing Beijing 100083 PR China

Low hydrogen evolution efficiency and poor conductivity hinder the application of layered hydroxide in overall water splitting. In this work, a CoNiFe- layered ternary hydroxide heterostructure with Co 9 S 8 quantum dot (CoNiFe-LTH/Co 9 S 8 QDs) intercalation was ingeniously designed by using in-situ selective vulcanization and laminar confinement effect. CoNiFe-LTH/Co 9 S 8 QDs exhibits excellent hydrogen evolution reaction (HER), oxygen evolution reaction (OER) and bifunctional electrocatalytic activities in alkaline media. The assembled alkaline electrolyzer requires only 1.59 V to achieve a current density of 100 mA cm −2 and demonstrates brilliant durability for over 80 hours. With the aid of electrochemical impedance spectroscopy and theoretical calculations, it is verified that the interlayer Co 9 S 8 QDs enhance the electron transfer the adsorption of H 2 O between LTH layers, resulting in a great improvement in HER performance. For OER, Co 9 S 8 QDs promote the transformation of CoNiFe-LTH to highly valent active species, while oxygen vacancies (Ov) created by in-situ selective sulfidation as new OH - adsorption activity centers, increasing the intrinsic OER activity of CoNiFe-LTH. Overall, this work provides new inspiration for the rational design of non-precious metal-based bifunctional electrocatalysts.

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Covalent-organic frameworks with keto-enol tautomerism for efficient photocatalytic oxidative coupling of amines to imines under visible light

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Science China Chemistry 2021年第12期64卷 2169-2179页

作者： Zhenyu Wu Xiubing Huang Xiangjun Li Guangtong Hai Baozhen Li Ge Wang Beijing Advanced Innovation Center for Materials Genome Engineering Beijing Key Laboratory of Function Materials for Molecule&Structure ConstructionSchool of Materials Science and EngineeringUniversity of Science and Technology BeijingBeijing100083China

Photocatalytic oxidation of organic molecules into highly value-added products is an innovative and challenging research which has gradually attracted remarkable attention of *** this work,it is demonstrated that the COF-TpPa with keto-enol tautomerism equilibrium structure shows excellent performance(yield>99%after 8 h)in the selective photocatalytic oxidative coupling of amines to imines under visible light *** is revealed that three kinds of reactive oxygen species(superoxide radical,hydroxyl radical and singlet oxygen)participate in this photocatalytic oxidation *** addition,hydrogen protons cleaved from the benzyl are proven to be reduced to hydrogen in the conduction band of COF-TpPa in anaerobic atmosphere,accompanied with the formation of *** direct hydrogen evolution from amine provides an effective way to extract clean energy from organic molecule as well as the production of value-added *** a contrast,COF-LZU1 with similar structure and chemical composition to COF-TpPa but without keto-enol tautomerism exhibits worse optical properties and photocatalytic *** is also demonstrated that keto-enol tautomerism favors the adsorption of benzylamine based on the characterization results and theoretical calculations.

关键词： covalent-organic frameworks photocatalysts aerobic/anaerobic benzylamine oxidation keto-enol tautomerism

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