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strong metal–support interaction boosts the electrocatalytic hydrogen evolution capability of Ru nanoparticles supported on titanium nitride

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Carbon Energy 2024年第1期6卷 245-254页

作者： Xin Wang Xiaoli Yang Guangxian Pei Jifa Yang Junzhe Liu Fengwang Zhao Fayi Jin Wei Jiang Haoxi Ben Lixue Zhang College of Chemistry and Chemical Engineering Collaborative Innovation Center for Hydrogen Energy Key Materials and Technologies of Shandong ProvinceQingdao UniversityQingdaoShandongChina State Key Laboratory of Bio-fibers and Eco-Textiles Qingdao UniversityQingdaoShandongChina Qingdao Institute of Bioenergy and Bioprocess Technology Chinese Academy of ScienceQingdaoShandongChina

Ruthenium(Ru)has been regarded as one of the most promising alternatives to substitute Pt for catalyzing alkaline hydrogen evolution reaction(HER),owing to its inherent high activity and being the cheapest platinum-group metal.Herein,based on the idea of strong metal–support interaction(SMSI)regulation,Ru/TiN catalysts with different degrees of TiN overlayer over Ru nanoparticles were fabricated,which were applied to the alkaline electrolytic water.Characterizations reveal that the TiN overlayer would gradually encapsulate the Ru nanoparticles and induce more electron transfer from Ru nanoparticles to TiN support by the Ru–N–Ti bond as the SMSI degree increased.Further study shows that the exposed Ru–TiN interfaces greatly promote the H_(2) desorption capacity.Thus,the Ru/TiN-300 with a moderate SMSI degree exhibits excellent HER performance,with an overpotential of 38 mV at 10 mA cm^(−2).Also,due to the encapsulation role of TiN overlayer on Ru nanoparticles,it displays super long-term stability with a very slight potential change after 24 h.This study provides a deep insight into the influence of the SMSI effect between Ru and TiN on HER and offers a novel approach for preparing efficient and stable HER electrocatalysts through SMSI engineering.

关键词： electronic structure hydrogen evolution reaction ruthenium strong metal-support interaction titanium nitride

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Exploration of strong metal-support interaction in Heterogeneous Catalysts by in situ Transmission Electron Microscopy

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Chinese Journal of Chemistry 2024年第9期42卷 1004-1008页

作者： Yongjun Jiang Sheng Dai Key Laboratoryfor Advanced Materials and Feringa Nobel Prize Scientist Joint Research Center Institute of Fine ChemicalsSchool of Chemistry&Molecular EngineeringEast China Universityof Science and TechnologyShanghai 200237China

The phenomenon of strong metal-support interaction(SMSI)observed in supported metal catalysts,usually accompanied by the formation of the encapsulation layer on metal nanoparticles,has attracted extensive research attention due to its significance in heterogeneous catalysis.Notably,great progress has been made in recent years in investigating SMSI by in situ transmission electron microscopy(TEM),along with an enhanced comprehension of the underlying mechanisms governing SMSI formation.This emerging topic summarizes recent progress utilizing in situ TEM to study the interaction between metal and support and the relationship between the structure and performance of the supported catalyst under reaction conditions.A brief perspective about the use of in situ TEM for further study of SMSI is also presented,showing prospects in this field that will stimulate further upsurging research in promoting the catalytic efficiency of supported catalysts.

关键词： Heterogeneous catalysis In situ TEM strong metal-support interaction Structure changes Interfaces Structural evolution

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Investigating the impact of dynamic structural changes of Au/rutile catalysts on the catalytic activity of CO oxidation

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Carbon Energy 2024年第4期6卷 222-232页

作者： Xiaochun Hu Qianwenhao Fan Mingwu Tan Yuqing Luo Xianyue Wu Manoel Y.Manuputty Jie Ding Tej SChoksi Markus Kraft Rong Xu Zhiqiang Sun Wen Liu School of Energy Science and Engineering Central South UniversityChangshaChina School of Chemistry Chemical Engineering and BiotechnologyNanyang Technological UniversitySingaporeSingapore Cambridge Centre for Advanced Research and Education SingaporeSingapore Institute of Sustainability for Chemicals Energy and EnvironmentJurong IslandSingapore College of Chemistry and Chemical Engineering Central South UniversityChangshaChina Department of Chemical Engineering and Biotechnology University of CambridgeCambridgeUK

The surface properties of oxidic supports and their interaction with the supported metals play critical roles in governing the catalytic activities of oxide‐supported metal catalysts.When metals are supported on reducible oxides,dynamic surface reconstruction phenomena,including strong metal–support interaction(SMSI)and oxygen vacancy formation,complicate the determination of the structural–functional relationship at the active sites.Here,we performed a systematic investigation of the dynamic behavior of Au nanocatalysts supported on flame‐synthesized TiO_(2),which takes predominantly a rutile phase,using CO oxidation above room temperature as a probe reaction.Our analysis conclusively elucidated a negative correlation between the catalytic activity of Au/TiO_(2) and the oxygen vacancy at the Au/TiO_(2) interface.Although the reversible formation and retracting of SMSI overlayers have been ubiquitously observed on Au/TiO_(2) samples,the catalytic consequence of SMSI remains inconclusive.Density functional theory suggests that the electron transfer from TiO_(2) to Au is correlated to the presence of the interfacial oxygen vacancies,retarding the catalytic activation of CO oxidation.

关键词： CO oxidation electronic metal-support interactions flame‐synthesis metal-support interactions oxygen vacancy strong metal-support interaction

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Light-enhanced metal-support interaction for synergetic photo/thermal catalytic formaldehyde oxidation

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Journal of Materials Science & Technology 2023年第36期167卷 74-81页

作者： Jiawei Ye Linxi Wang Bicheng Zhu Bei Cheng Rongan He Laboratory of Solar Fuel Faculty of Materials Science and ChemistryChina University of GeosciencesWuhan 430078China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China Hunan Key Laboratory of Applied Environmental Photocatalysis Changsha UniversityChangsha 410022China

The strong metal-support interaction(SMSI)plays a pivotal role in regulating electronic properties and activating surface oxygen species.In this work,we report light-irradiation-modulated SMSI for enhanced formaldehyde(HCHO)oxidation.Specifically,the SMSI between Pt nanoparticles(NPs)and Bi_(2)MoO_(6)cre-ated surface-active oxygen at Pt-Bi_(2)MoO_(6)interfaces to activate HCHO to dioxymethylene(DOM).Notably,light irradiation boosted the SMSI and catalytic activity.Moreover,photogenerated holes in Bi_(2)MoO 6 im-proved HCHO adsorption and activation,while photogenerated electrons migrated from Bi_(2)MoO_(6)to Pt NPs to promote O_(2)adsorption and activation,accelerating the oxidation of DOM to CO_(2)and H_(2)O.The light-modulated SMSI and the synergy between photocatalysis and thermocatalysis lead to enhanced cat-alytic oxidation activity,providing a practical strategy for indoor volatile organic compound(VOC)de-composition under ambient conditions.

关键词： Formaldehyde oxidation strong metal-support interaction Photocatalysis Photo-thermal synergy Electron transfer

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Precious metal-support interaction in automotive exhaust catalysts

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Journal of Rare Earths 2014年第2期32卷 97-107页

作者：郑婷婷何俊俊赵云昆夏文正何洁丽 State-Local Joint Engineer Laboratory of Precious metal Catalytic Technology and Application Kunming Sino-platinum Metals Catalysts Co. Ltd. State Key Laboratory of Advanced Technologies for Comprehensive Utilization of Platinum metals Kunming Institute of Precious Metals

Precious metal-support interaction plays an important role in thermal stability and catalytic performance of the automotive exhaust catalysts. The support is not only a cartier for active compotmds in catalysts but also can improve the dispersion of precious metals and suppress the sintering of precious metals at high temperature; meanwhile, noble metals can also enhance the redox performance and oxygen storage capacity of support. The mechanism of metal-support interactions mainly includes electronic interaction, formation of alloy and inward diffusion of metal into the support or covered by support. The form and degree of precious metal-sup- port interaction depend on many factors, including the content of precious metal, the species of support and metal, and preparation methods. The research results about strong metal-support interaction （SMSI） gave a theory support for developing a kind of new cata- lyst with excellent performance. This paper reviewed the interaction phenomenon and mechanism of precious metals （Pt, Pd, Rh） and support such as A1203, CeO2, and CeO2-based oxides in automotive exhaust catalysts. The factors that affect SMSI and the catalysts developed by SMSI were also discussed.

关键词： strong metal-support interaction automotive exhaust catalyst precious metal Al2O3 CeO2-based oxides rare earths

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Low temperature one-pot synthesis of 1,1-diethoxyethane from ethanol on Bi/BiCeO_(x)with strong metal-support interactions

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Nano Research 2023年第3期16卷 3709-3718页

作者： Zhe An Jiayu Liu Meng Cao Jian Zhang Yanru Zhu Hongyan Song Xu Xiang Jing He State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical TechnologyBeijing 100029China

The direct conversion of ethanol to 1,1-diethoxyethane(DEE)through one-pot dehydrogenation-acetalization has attracted broad interest from both academia and industry.Based on thermodynamics,the oxidative dehydrogenation of alcohol to acetaldehyde requires high temperature to activate oxygen to realize the C-H cleavage,while the acetalization of acetaldehyde with ethanol is exothermic reversible reaction favorable at low temperature.The mismatching of the reaction condition for the two consecutive steps makes it a great challenge to achieve both high ethanol conversion and high DEE selectivity.This work reports a highly efficient bi-functional catalysis by Bi/BiCeO_(x)for one-pot oxidative dehydrogenation-acetalization route from ethanol to DEE under 150℃and ambient pressure,affording a selectivity of 98.5%±0.5%to DEE at an ethanol conversion of 87.0%±1.0%.An efficient tandem catalysis has been achieved on the interfacial Bi^(δ)+-Ov-Ce^(III)sites in Bi/BiCeO_(x)established by strong metal-support interaction,in which Biδ+-Ov-sites contribute to the oxidative dehydrogenation of ethanol at mild temperature,and-Ov-CeIII sites to the subsequent acetalization between the generated acetaldehyde and ethanol.

关键词： ethanol conversion 1 1-diethoxyethane strong metal-support interaction Biδ+-Ov-CeIII sites

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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 reactions.However,the sintering and/or leaching of metal NPs occurred under harsh reaction conditions that caused the catalyst deactivation.strong metal-support interactions(SMSIs)serve as an effective method to stabilize the metal NPs against sintering and leaching,which have been extensively studied.In 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 performances.In this review,we briefly summarize these routes that avoid the high-temperature reduction treatments for the construction of SMSIs.Their significant advantages in stabilizing metal NPs,modulating the geometric/electronic structure of metal species,and the mechanism on the SMSI formation are particularly discussed.Finally,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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Direct environmental TEM observation of silicon diffusion-induced strong metal-silica interaction for boosting CO_(2)hydrogenation

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Nano Research 2023年第2期16卷 2209-2217页

作者： Lei Wang Lei Zhang Luyao Zhang Yulong Yun Kun Wang Boyuan Yu Xin Zhao Feng Yang Department of Chemistry Southern University of Science and TechnologyShenzhen 518055China

For the high-temperature catalytic reaction,revealing the interface of catalyst–support and its evolution under reactive conditions is of crucial importance for understanding the reaction mechanism.However,much less is known about the atomic-scale interface of the hard-to-reduce silica-metal compared to that of reducible oxide systems.Here we reported the general behaviors of SiO_(2)migration onto various metal(Pt,Co,Rh,Pd,Ru,and Ni)nanocrystals supported on silica.Typically,the Pt/SiO_(2)catalytic system,which boosted the CO_(2)hydrogenation to CO,exhibited the reduction of Si0 at the Pt-SiO2 interface under H2 and further Si diffusion into the near surface of Pt nanoparticles,which was unveiled by in-situ environmental transmission electron microscopy coupled with spectroscopies.This reconstructed interface with Si diffused into Pt increased the sinter resistance of catalyst and thus improved the catalytic stability.The morphology of metal nanoparticles with SiO_(2)overlayer were dynamically evolved under reducing,vacuum,and oxidizing atmospheres,with a thicker SiO_(2)layer under oxidizing condition.The theoretical calculations revealed the mechanism that the Si-Pt surface provided synergistic sites for the activation of CO_(2)/H_(2)to produce CO with lower energy barriers,consequently boosting the high-temperature reverse water-gas shift reaction.These findings deepen the understanding toward the interface structure of inert oxide supported catalysts.

关键词： in-situ environmental transmission electron microscopy interface strong metal-support interaction silica support reverse water gas-shift reaction

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Engineering titanium oxide-based support for electrocatalysis

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Journal of Energy Chemistry 2022年第4期31卷 168-183页

作者： Ke Chen Tao Shen Yun Lu Yezhou Hu Jingyu Wang Jian Zhang Deli Wang Key Laboratory of Material Chemistry for Energy Conversion and Storage(Huazhong University of Science and Technology) Ministry of EducationHubei Key Laboratory of Material Chemistry and Service FailureSchool of Chemistry and Chemical EngineeringHuazhong University of Science and TechnologyWuhan 430074HubeiChina

The corrosion and weaker interaction with metal catalysts of common carbon supports during electrocatalysis push the development of alternative supports materials. Titanium oxide-based materials have been widely explored as electrocatalysts supports in consideration of their chemical stability, strong interactions with metal catalyst and wider applications in electrocatalytic reactions as well as the improved electronic conductivity. This review summarizes recent research advances in engineering titanium oxide-based supports for the catalysts in electrocatalysis field to provide guidance for designing high performance non-carbon supported electrocatalysts. Typically, the titanium oxide-based supports are classified into shaped TiO_(2), doped TiO_(2), titanium suboxide and TiO_(2)-carbon composites according to the modification methods and corresponding preparation methods. Then the engineering strategies and electrocatalytic applications are discussed in detail. Finally, the challenges, future research directions and perspectives of titanium oxide-based supports for electrocatalysis are presented for practical applications.

关键词： Titanium oxide support Electrocatalysis strong metal-support interaction Electrochemical reactions

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Bulky nanodiamond-confined synthesis of sub-5 nanometer ordered intermetallic Pd_(3)Pb catalysts

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Nano Research 2022年第6期15卷 4973-4979页

作者： Lei Wang Peng Yin Wei-Jie Zeng Shi-Long Xu Ping Chen Hai-Wei Liang Department of Chemistry University of Science and Technology of ChinaHefei 230026China School of Chemistry and Chemical Engineering Anhui UniversityHefei 230601China

Modulation of geometric and electronic structures of supported Pd-based catalysts by forming atomically ordered intermetallic phases enables an effective way to optimize catalytic performance.However,the synthesis of small-sized Pd-based intermetallic nanoparticle catalysts with improved mass-based activity remains formidable challenges,since high-temperature annealing generally required for atom ordering inevitably leads to severe metal sintering and thus large crystallites.Here,we present a bulky nanodiamond-confined method to prepare sub-5 nm Pd_(3)Pb intermetallic nanocatalysts by mitigating metal sintering at high temperatures,which is induced by the electronic interactions between metal and defect-rich graphene shells reinforced by diamond cores in the bulky nanodiamond support.The prepared small-sized Pd_(3)Pb intermetallic catalyst displays a high activity with a turnover frequency of 932 h−1 for the semihydrogenation of phenylacetylene under mild conditions(room temperature,3 bar H_(2)),along with a high selectivity of>96%to styrene near the complete conversion of phenylacetylene.

关键词： Pd_(3)Pb intermetallic compound bulky nanodiamond strong metal-support interaction alkynes semihydrogenation

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