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Tunable hydrogen coverage on electron-deficient platinum nanoparticles for efficient hydrogenation reactions

Nano Research 2023年第7期16卷 8751-8756页

作者： Lu-Han Sun Qi-Yuan Li Yu-Shuai Xu Si-Yuan Xia Dong Xu Xiu Lin Jingsan Xu Jie-Sheng Chen Guo-Dong Li Xin-Hao Li School of Chemistry and Chemical Engineering Frontiers Science Center for Transformative MoleculesShanghai Jiao Tong UniversityShanghai 200240China School of Chemistry and Physics Faculty of ScienceCentre for Materials ScienceQueensland University of TechnologyBrisbaneQLD 4001Australia State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of ChemistryJilin UniversityChangchun 130012China

Dissociation of active H species over the catalytic sites with the carbon-supported Pt metals as the mainstream catalysts is crucial to facilitate hydrogen donation and accelerate the hydrogen addition process in catalytic hydrogenation systems to produce polymers,pharmaceuticals,agrochemicals,fragrances,and biofuels at million-ton *** attention has been paid to the design of the more active catalytic site to effectively adsorb and activate reactants and H_(2) *** the same time,there is still a huge room to develop powerful strategies to accelerate the donation of acted H species to the reactants from the Pt surface further to boost the final catalytic efficiencies of Pt catalysts and depress the total Pt ***,we present a new strategy for promoting the Pt-H bond dissociation by increasing surface hydrogen coverage on designed electron-deficient Pt *** electron deficiency of Pt nanoparticles has been successfully tuned by constructing a rectifying contact with an even“noble”boron-rich carbon support(Pt/BC).Theoretical and experimental results confirm the dominant role of the pronounced electron deficiencies of Pt nanoparticles in enhancing the H coverage for 2.3 times higher than that of neutral Pt nanoparticles,significantly boosting the Pt-H bond dissociation and thus the whole hydrogenation process as reflected by the extremely high turnover frequency(TOF)value of 388 h^(-1)at 30℃ and 10 bar H_(2) for phenol hydrogenation on the Pt/BC,outperforming the bench-marked catalysts by a factor of 9.

关键词： hydrogenation hydrogen coverage Schottky barrier heterogeneous catalysis

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A multi-functional Ru Mo bimetallic catalyst for ultra-efficient C3 alcohols production from liquid phase hydrogenolysis of glycerol

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Chinese Journal of Chemical Engineering 2022年第11期51卷 199-215页

作者： Guoxiao Cai Wei Xiong Susu Zhou Pingle Liu Yang Lv Fang Hao Hean Luo ChangYi Kong College of Chemical Engineering National&Local United Engineering Research Centre for Chemical Process Simulation and IntensificationXiangtan UniversityXiangtan 411105China Department of Environment and Energy System Graduate School of Science and TechnologyShizuoka University3-5-1 JohokuNaka-kuHamamatsu 432-8561Japan

Ru and Mo bimetallic catalysts supported on active carbon modified by phosphotungstic acid(PW)were designed and applied in glycerol hydrogenolysis *** physicochemical properties of the catalysts were characterized and the presence of active sites was investigated from the perspective of the glycerol hydrogenolysis *** MoOxis highly selective for the C—O bond cleavage of glycerol molecules,which can reasonably regulate the strong C—C bond cleavage activity of Ru *** using sequential deposition of Ru and Mo supported on mesoporous PW-C,the characterization results show that the combination of isolated low-valence MoOxwith metal Ru particles can form“MoOx-Ru-PW”,which provides highly catalytic activity toward C—O bond cleavage,selectively producing more C3 alcohols(mainly 1,2(3)-propanediol).The glycerol conversion of 1%Mo/Ru/PW-C catalyst was 59.6%,the selectivity of C3 alcohol was 96.1%,and the selectivity of propanediol(1,2(3)-propanediol)was 94.9%.It is noteworthy that the selectivity of 1,3-propanediol reached 20.7%when the PW was 21.07%(mass).This study provides experimental evidence for the tandem dehydration and hydrogenation mechanism of the multifunctional Mo/Ru/PW-C catalyst.

关键词： heterogeneous catalysis Bimetallic catalyst Glycerol hydrogenolysis Ruthenium Molybdenum Phosphotungstic acid

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Catalytically active atomically thin cuprate with periodic Cu single sites

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National Science Review 2023年第1期10卷 226-235页

作者： Huimin Yang Shibo Xi Na Guo Mu Wang Lingmei Liu Pin Lyu Xiaolong Yu Jing Li Haomin Xu Xiao Hai Zejun Li Xinzhe Li Tao Sun Xiaoxu Zhao Yu Han Wei Yu Jie Wu Chun Zhang Honghan Fei Ming Joo Koh Jiong Lu Department of Chemistry National University of Singapore Institute of Chemical and Engineering Sciences Department of Physics National University of Singapore Advanced Membranes and Porous Materials Center King Abdullah University of Science and Technology SDU-ANU Joint Science College Shandong University School of Materials Science and Engineering Peking University Centre for Advanced 2D Materials and Graphene Research Centre National University of Singapore Department of Chemistry Tongji University

Rational design and synthesis of catalytically active two-dimensional(2D) materials with an abundance of atomically precise active sites in their basal planes remains a great ***,we report a ligand exchange strategy to exfoliate bulk [Cu4(OH)6] [O3S(CH2)4SO3] cuprate crystals into atomically thin 2D cuprate layers([Cu2(OH)3]+).The basal plane of 2D cuprate layers contains periodic arrays of accessible unsaturated Cu(Ⅱ) single sites(2D-CuSSs),which are found to promote efficient oxidative Chan-Lam *** me chanistic studies reveal that the reactions proceed via coordinatively unsaturated CuO4(Ⅰ) single sites with the formation of Cu(Ⅰ) species in the rate-limiting step,as corroborated by both operando experimental and theoretical *** robust stability of 2D-CuSSs in both batch and continuous flow reactions,coupled with their recyclability and good performance in complex molecule derivatization,render 2D-CuSSs attractive catalyst candidates for broad utility in fine chemical synthesis.

关键词： exfoliation nanosheet heterogeneous catalysis

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New routes for the construction of strong metal-support interactions

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Science China Chemistry 2022年第11期65卷 2051-2057页

作者： Hai Wang Liang Wang Feng-Shou Xiao Key Lab of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological EngineeringZhejiang UniversityHangzhou310027China College of Chemistry Zhengzhou UniversityZhengzhou 450001China

Supported metal nanoparticles(NPs)on solid carriers are highly efficient catalysts in many industrial ***,the sintering and/or leaching of metal NPs occurred under harsh reaction conditions that caused the catalyst *** metal-support interactions(SMSIs)serve as an effective method to stabilize the metal NPs against sintering and leaching,which have been extensively *** addition to the classical route to construct SMSIs via high-temperature reduction treatments,new routes have emerged recently to extend the scope of catalysts with SMSIs and optimized their catalytic *** this review,we briefly summarize these routes that avoid the high-temperature reduction treatments for the construction of *** significant advantages in stabilizing metal NPs,modulating the geometric/electronic structure of metal species,and the mechanism on the SMSI formation are particularly ***,the current challenges and developing trends in the construction of SMSIs for achieving more efficient catalysts are outlooked.

关键词： strong metal-support interaction supported catalyst metal nanoparticles heterogeneous catalysis

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Fully-exposed Pt clusters stabilized on Sn-decorated nanodiamond/graphene hybrid support for efficient ethylbenzene direct dehydrogenation

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Nano Research 2022年第12期15卷 10029-10036页

作者： Linlin Wang Xuetao Qin Ting Sun Xiangbin Cai Mi Peng Zhimin Jia Xiaowen Chen Ning Wang Jiangyong Diao Hongyang Liu Ding Ma Department of Chemistry Northeastern UniversityShenyang110819China Shenyang National Laboratory for Materials Science Institute of Metal ResearchChinese Academy of SciencesShenyang110016China Beijing National Laboratory for Molecular Engineering College of Chemistry and Molecular Engineering and College of EngineeringBIC-ESATPeking UniversityBeijing100871China Department of Physics Hong Kong University of Science and TechnologyKowloonHong Kong999077China School of Materials Science and Engineering University of Science and Technology of ChinaHefei230026China

The pursuit of energy conservation and environmental protection has always been a hot topic in the catalytic fields,which is inseparable from the rational designing of efficient catalysts and an in-depth understanding of the catalytic reaction *** this work,fully-exposed Pt clusters were fabricated on the atomically dispersed Sn decorated nanodiamond/graphene(Sn-ND@G)hybrid support and employed for direct dehydrogenation(DDH)of ethylbenzene(EB)to styrene(ST).The detailed structural characterizations revealed the fully-exposed Pt clusters were stabilized on Sn-ND@G,assisted by the spatial separation of atomically dispersed Sn *** as-prepared Pt/Sn-ND@G catalyst showed enhanced ST yield(136.2 molEB·molpt-1·h-1 EB conversion rate and 99.7%ST selectivity)and robust long-term stability at 500℃for the EB DDH reaction,compared with the traditional ND@G supported Pt nanoparticle catalyst(Pt/ND@G).The ST prefers to desorb from the fully-exposed Pt clusters,resulting in the enhanced DDH catalytic performance of the Pt/Sn-ND@G *** present work paves a new way for designing highly dispersed and stable supported metal catalysts for DDH reactions.

关键词： Pt cluster ethylbenzene dehydrogenation fully-exposed catalyst heterogeneous catalysis

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Mesoporous poly(ionic liquid)s with dual active sites for highly efficient CO_(2)conversion

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Green Energy & Environment 2023年第2期8卷 478-486页

作者： Yawen Fu Yanan Xu Zepeng Zeng Abdul-Rauf Ibrahim Jin Yang Shuliang Yang Yaqiang Xie Yanzhen Hong Yuzhong Su Hongtao Wang Yanliang Wang Li Peng Jun Li Wendy L.Queen College of Chemistry and Chemical Engineering Xiamen UniversityXiamen361005China Mechanical Engineering Department Tamale Technical UniversityTamaleGhana College of Energy Xiamen UniversityXiamen361102China National Engineering Laboratory for Green Chemical Productions of Alcohols Ethers and EstersXiamen UniversityXiamen361005China Collaborative Innovation Center of Chemistry for Energy Materials Xiamen361005China Institute of Chemical Sciences and Engineering Ecole Polytechnique Federale de Lausanne(EPFL)EPFL-ISIC-ValaisSionSwitzerland

Atmospheric CO_(2)concentrations are soaring due to the continued use of fossil fuels in energy production,an anthropogenic activity that is playing a leading role in global ***,research aimed at the capture and conversion of CO_(2)into value-added products,such as cyclic carbonates,is *** CO_(2)is an abundant,cheap,non-toxic,and readily accessible Cl feedstock,its thermodynamic stability necessitates the development of highly efficient catalysts that are able to promote chemical reactions under mild *** this work,a novel mesoporous poly(ionic liquid)with dual active sites was synthesized through a facile method that involves co-polymerization,post-synthetic metalation,and supercritical CO_(2)*** to a high density of nucleophilic and electrophilic sites,the as-prepared poly(ionic liquid),denoted as P2D-4BrBQA-Zn,offers excellent performance in a CO_(2)cycloaddition reaction using epichlorohydrin as the substrate(98.9%conversion and 96.9%selectivity).Moreover the reaction is carried out under mild,solvent-free,and additive-free ***,P2D-4BrBQA-Zn also efficiently promotes the conversion of various other epoxide substrates into cyclic ***,the catalyst is found to have excellent substrate compatibility,stability,and recyclability.

关键词： Mesoporous poly(ionic liquid) Nucleophile/electrophilic sites Carbon dioxide cycloaddition heterogeneous catalysis Supercritical CO_(2)drying

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Use of catalytic wet air oxidation (CWAO) for pretreatment of high-salinity high-organic wastewater

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Journal of Environmental Sciences 2022年第10期34卷 105-114页

作者： Wenjing Sun Hongxia Lv Lei Ma Xiangdong Tan Chengyu Jin Huiling Wu Lili Chen Mengyang Liu Huangzhao Wei Chenglin Sun Dalian Institute of Chemical Physics Chinese Academy of SciencesDalian 116023China Beijing Key Laboratory of Fuels Cleaning and Advanced Catalytic Emission Reduction Technology College of Chemical EngineeringBeijing Institute of Petrochemical TechnologyBeijing 102617China University of Chinese Academy of Sciences Beijing 100049China

Catalytic wet air oxidation(CWAO)coupled desalination technology provides a possibility for the effective and economic degradation of high salinity and high organic *** widely occurs in natural and wastewaters,and its high content jeopardizes the efficacy of Advanced oxidation process(AOPs).Thus,a novel chlorine ion resistant catalyst Bsite Ru doped LaFe_(1-x)Ru_(x)O_(3-)δin CWAO treatment of chlorine ion wastewater was ***,LaFe_(0.85)Ru_(0.15)O_(3-δ)was 45.5% better than that of the 6%RuO_(2)@TiO_(2)(commercial carrier)on total organic carbon(TOC)***,doped catalysts LaFe_(1-x)Ru_(x)O_(3-)δshowed better activity than supported catalysts RuO_(2)@LaFeO_(3) and RuO_(2)@TiO_(2) with the same Ru ***,LaFe_(0.85)Ru_(0.15)O_(3-)δhas novel chlorine ion resistance no matter the concentration of Cl^(−) and no Ru dissolves after the reaction.X-ray diffraction(XRD)refinement,X-ray photoelectron spectroscopy(XPS),transmission electron microscope(TEM),and X-ray absorption fine structure(XAFS)measurements verified the structure of LaFe_(0.85)Ru_(0.15)O_(3-)δ.Kinetic data and density functional theory(DFT)proved that Fe is the site of acetic acid oxidation and adsorption of chloride *** existence of Fe in LaFe_(0.85)Ru_(0.15)O_(3-)δcould adsorb chlorine ion(catalytic activity inhibitor),which can protect the Ru site and other active oxygen species to exert catalytic *** work is essential for the development of chloride-resistant catalyst in CWAO.

关键词： Catalytic wet air oxidation heterogeneous catalysis LaFe_(1-x)Ru_(x)O_(3-)δ Chlorine wastewater Salt resistance mechanism

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Efficient homogenous catalysis of CO_(2) to generate cyclic carbonates by heterogenous and recyclable polypyrazoles

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Chinese Journal of Chemical Engineering 2022年第3期35卷 110-115页

作者： Zhen Lu Jie He Bogeng Guo Yulai Zhao Jingyu Cai Longqiang Xiao Linxi Hou Department of Materials-Oriented Chemical Engineering School of Chemical EngineeringFuzhou UniversityFuzhou 350116China Qingyuan Innovation Laboratory Quanzhou 362801China Fujian Key Laboratory of Advanced Manufacturing Technology of Specialty Chemicals Fuzhou UniversityFuzhou 350116China

The cycloaddition between CO_(2)and epoxides to produce cyclic carbonate is an attractive and efficiency pathway for the utilization of CO_(2)as C1 *** development of catalyst to mediate cycloaddition between CO_(2)and epoxides at low temperature and pressure is still a ***,a series of polypyrazoles with glass transition temperature(T_(g))in the range of 42.3-52.5℃ were synthesized and served as catalyst to mediate the cycloaddition of CO_(2)and epoxides by the assistant of tetrabutylammonium *** catalytic behaviors of polypyrazole on the model cycloaddition of CO_(2)to epichlorohydrin,including the reaction parameters optimization and versatility were investigated in detail,and excellent yield(99.9%)and selectivity(99%)were obtained under the optimized reaction conditions of70℃ and 1.0 MPa for 6.0 ***,the polypyrazole acts as homogeneous catalyst during reaction(higher than T_(g)).And under room temperature,polypyrazoles can be easily separated and recovered,which is a promising feature of a heterogeneous ***,the reaction mechanism was *** DFT calculation suggested that the formation of hydrogen bond between pyrazole and epoxide greatly reduced the energy barrier,which play an important role in promoting CO_(2)cycloaddition.

关键词： Carbon dioxide CO_(2)conversion Cyclic carbonate heterogeneous catalysis Polypyrazole

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Spatial compartmentalization of metal nanoparticles within metal-organic frameworks for tandem reaction

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Nano Research 2022年第2期15卷 1178-1182页

作者： Ting Pan Islam E.Khalil Zhiling Xu Hongfeng Li Xinglong Zhang Gengwu Xiao Weina Zhang Yu Shen Fengwei Huo Key Laboratory of Flexible Electronics(KLOFE)and Institute of Advanced Materials(IAM) Nanjing Tech UniversityNanjing 211816China

Fabrication of multifunctional catalysts has always been the pursuit of synthetic chemists due to their efficiency,cost-effectiveness,and environmental ***,it is difficult to control multi-step reactions in one-pot,especially the spatial compartmentalization of incompatible active ***,we constructed metal-organic framework(MOF)composites which regulate the location distribution of metal nanoparticles according to the reaction path and coupled with the diffusion of substrates to achieve tandem *** designed UiO-66-Pt-Au catalyst showed good activity and selectivity in hydrosilylation-hydrogenation tandem reaction,because the uniform microporous structures can control the diffusion path of reactants and intermediates,and Pt and Au nanoparticles were arranged in core-shell spatial distribution in *** contrast,the low selectivity of catalysts with random deposition and physical mixture demonstrated the significance of artificial control to the spatial compartmentalization of active sites in tandem catalytic reactions,which provides a powerful approach for designing high-performance and multifunctional heterogeneous catalysts.

关键词： metal-organic frameworks metal nanoparticles spatial compartmentalization tandem reaction heterogeneous catalysis

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Oxygen/Sulfur Atom Exchange Copolymerization of Carbon Disulfide and Propylene Oxide by a Highly Effective heterogeneous Berlin Green Catalyst

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Chemical Research in Chinese Universities 2023年第5期39卷 790-796页

作者： Munir Ullah KHAN Safir Ullah KHAN CAO Xiaohan Muhammad USMAN Muhammad Naeem SHAH Abdul GHAFFAR Muhammad HASSAN ZHANG Chengjian ZHANG Xinghong State Key Laboratory of Motor Vehicle Biofuel Technology International Research Center for X PolymersDepartment of Polymer Science and EngineeringZhejiang UniversityHangzhou 310027P.R.China Shanxi-Zheda Institute of Advanced Materials and Chemical Engineering Shanxi 030013P.R.China Hefei National Laboratory for Physical Science at the Microscale School of Life SciencesUniversity of Science and Technology of ChinaHefei 230027P.R.China Key Laboratory of Macromolecular Synthesis and Functionalization(Ministry of Education) International Research Center for X PolymersDepartment of Polymer Science and EngineeringZhejiang UniversityHangzhou 310027P.R.China College of Information Science and Electronic Engineering Zhejiang UniversityHangzhou 310027P.R.China Advanced Materials Research Center Zhejiang University-University of Illinois at Urbana-Champaign Institute(ZJU-UIUC)Haining 314400P.R.China

In this study,we report that Berlin Green(FeFe-BG)framework exhibits superior performance in the catalytic coupling of carbon disulfide(CS_(2))and propylene oxide(PO)to generate a random copolymer containing thioether,propylene monothiocarbonate and ether *** and sulfur atom exchange was detected in polymeric and cyclic thiocarbonate byproducts and utilized to modulate the copolymerization of CS_(2)and propylene *** coupling of PO and CS_(2)was selective for copolymer formation under various reaction conditions.^(1)H and^(13)C NMR spectroscopy determined two distinct polymer linkages and two cyclic *** number average molecular weights ranged from 6.4 kg/mol to 10.5 kg/mol,with a comparatively low polydispersity of *** CS_(2)/PO molar feed ratio had a significant impact on the O/S exchange process;the ratio of cyclic thiocarbonate byproducts could be efficiently regulated by tuning the CS_(2)molar feed ratio.

关键词： Carbon disulfide Copolymerization Prussian Blue analogue heterogeneous catalysis Berlin Green

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