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Modulation effects of Cu modification and ligands (oxalate and borohydride) functionalization on Pt d-band center, upper d-band edge, and alloyed PtCe support acidity on semihydrogenation of acetylene

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Journal of Energy Chemistry 2022年第9期31卷 495-508,I0014页

作者： Olumide Bolarinwa Ayodele International Iberian Nanotechnology Laboratory Braga 4715-330Portugal Department of Civil and Chemical Engineering University of Tennessee ChattanoogaTN 37403United States

The modulating effects of Cu modification and oxalate or borohydride ligands functionalization on the structure,catalyst d-band center(εd),upper d-band edge(εu),and acetylene partial hydrogenation of expediently synthesized Ce alloyed Pt supported catalysts were ***,a 5 wt%Pt alloyed Ce was synthesized via flame spray *** PtCe sample was further supported on zeolite Y,ZY,(PtCe/ZY)and copper modified ZY(PtCe/Cu-ZY).Furthermore,the PtCe was supported on two other oxalate and borohydride ligands functionalized copper modified ZY(PtCe/CuX-ZY and PtCe/CuB-ZY,respectively).The high-angle annular darkfield scanning transmission electron microscopy(HAADF/STEM)data showed a reduction in the PtO average particle size from 2.65 nm in PtCeO_(2) to average 1.73,0.64,and 0.30 nm in PtCe/Cu-ZY,PtCe/CuX-ZY,and PtCe/CuB-ZY,which was corroborated by the electron energy-loss spectroscopy(EELS)results wherein nonhomogeneous mixing of elements was seen with segregated Pt clusters in the non-functionalized ***,both PtCe/CuX-ZY and PtCe/CuBZY samples showed near-perfect homogeneity with no distinct Pt *** measuredεu values for PtCe,PtCe/Cu-ZY,PtCe/CuX-ZY,and PtCe/CuB-ZY are+1.85,+0.40,-0.15,and-0.19 eV,*** positive values indicated strong metal-adsorbate bonding typical of large Pt sizes while the negative values indicated weak metal-adsorbate bonding due to highly downsized Pt *** ethylene yield(YC2H4)over the PtCe sample showed depletion as the reaction temperature increased,while it reflected maxima at 120℃ with 55.3%YC2H4 over PtCe/*** maxima shifted to 180℃ with enhanced YC2H4 of 71.4%in PtCe/*** the contrary,both PtCe/CuX-ZY and PtCe/CuB-ZY exhibited a monotonous increase in YC2H4 up to the maximum C_(2)H_(2)conversion with YC2H4 of 81.9%and 92.1%at 180 and 160℃,*** results showed that both the Cu modification and ligands functionalization were highly invaluable to enhance the properties and

关键词： Acetylene semihydrogenation Ethylene Pt d-band center Upper d-band edge

Acidic Electrocatalytic semihydrogenation of Alkynols to Alkenols on Copper Phosphide at Industrial-Level Current Density

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Chinese Journal of Chemistry 2023年第24期41卷 3618-3624页

作者： Sanyin Yang Jun Bu Rui Bai Jin Lin Siying An Yafei Wu Ying Guo Jie Gao Jian Zhang School of Chemistry and Chemical Engineering Northwestern Polytechnical UniversityXi'anShaanxi710129 China State Key Laboratory of Solidification Processing School of Materials Science and EngineeringNorthwestern Polytechnical UniversityXi'anShaanxi710072 China Interdisciplinary Research Center of Biology & Catalysis School of Life SciencesNorthwestern Polytechnical UniversityXi'anShaanxi710072 China

Alkenols are important intermediates for the industrial manufacture of various commodities and fine *** present,alkenols are produced via thermocatalytic semihydrogenation of corresponding alkynols using precious metal Pd-based catalysts in pressurized hydrogen *** this work,we highlight an efficient electrocatalytic strategy for selectively reducing alkynols to alkenols under ambient *** 2-methyl-3-butyn-2-ol as a model alkynol,Cu3P nanoarrays anchored on Cu foam remarkably deliver an industrial-level partial current density of 0.79 A·cm^(-2) and a specific selectivity of 98%for 2-methyl-3-buten-2-ol in acidic *** a 40-runs stability test,Cu3P nanoarrays maintain 90%alkynol conversion and 90%alkenol *** in a large two-electrode flow electrolyser,the single-pass alkynol conversion and alkenol selectivity of Cu3P nanoarrays exceed 90%.Moreover,this selective electrocatalytic hydrogenation approach is broadly feasible for the production of various water-soluble *** analyses,theoretical simulation and electrochemical in-situ infrared investigations together reveal that exothermic alkynol hydrogenation,facile alkenol desorption and formation of active H on Cu3P surfaces account for the excellent electrocatalytic performance.

关键词： Alkynol Alkenol Cu_(3)P nanoarrays Electrocatalysis semihydrogenation Mass spectrometry IR spectroscopy Heterogeneous catalysis

Cu_(2)O-SupportedAtomicallyDispersed Pd Catalysts for semihydrogenation of Terminal Alkynes: Critical Role of Oxide Supports

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CCS Chemistry 2019年第2期1卷 207-214页

作者： Kunlong Liu Ruixuan Qin Lingyun Zhou Pengxin Liu Qinghua Zhang Wentong Jing Pengpeng Ruan Lin Gu Gang Fu Nanfeng Zheng Collaborative Innovation Center of Chemistry for Energy Materials State Key Laboratory for Physical Chemistry of Solid Surfacesand Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Institute of Physics Chinese Academy of SciencesBeijing 100190China

Atomically dispersed catalysts have demonstrated superior catalytic performance in many chemical ***,limited success has been achieved in applying oxide-supported atomically dis-persed catalysts to semihydrogenation o... 详细信息

关键词： atomically dispersed catalyst support effect palladium semihydrogenation selective hydrogenation alkynes heterolytic activation of hydrogen galvanic displacement

Weak Acetylene Adsorption Terminated Carbon-Carbon Coupling Kinetics on Silver Electrocatalysts

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CCS Chemistry 2023年第1期5卷 200-208页

作者： Rui Bai Jinjin Li Jin Lin Zhenpeng Liu Chen Yan Lei Zhang Jian Zhang Key Laboratory of Special Functional and Smart Polymer Materials of Ministry of Industry and Information Technology School of Chemistry and Chemical EngineeringNorthwestern Polytechnical UniversityXi’anShaanxi 710129 State Key Laboratory of Solidification Processing and School of Materials Science and Engineering Northwestern Polytechnical UniversityXi’anShaanxi 710072

Owing to serious poison of downstream olefin polymerization catalysts from acetylene impurities,selective reduction of acetylene to ethylene is a pivotal process in petrochemical ***,during thermocatalytic and electrocatalytic acetylene semihydrogenation,acetylene C-C coupling inevitably occurs on current *** resultant oligomeric species(particularly long-chain hydrocarbons)block active sites and mass transportation,and eventually decrease catalytic activity and *** this work,we report Ag nanowires(NWs)as high-performance electrocatalysts for acetylene semihydrogenation,where the C-C coupling is unprecedentedly suppressed by weakening acetylene *** pure acetylene,1,3-butadiene Faradaic efficiency(FE)of Ag NWs is only 2.1%,which is far lower than 41.2%for Cu nanoparticles at−0.2 V versus reversible hydrsogen *** partial current density of Ag NWs reaches 217 mA/cm^(2)at 0.85 V,which is considerably higher than those for state-of-the-art Cu-based ***,no 1,3-butadiene is produced on Ag NWs in a large two-electrode flow cell fed with crude ethylene containing 1 vol%acetylene,presenting thorough termination of acetylene C-C *** situ electrochemical Raman spectroscopy and theoretical investigations reveal that weak acetylene adsorption on Ag surfaces is intrinsically responsible for prohibiting their *** work will spark the rapid development of high-performance and stable electrocatalysts for reducing alkynes to olefins.

关键词： acetylene electrocatalysis carbon-carbon coupling semihydrogenation silver nanowires

Single-atom Pd dispersed on nanoscale anatase TiO2 for the selective hydrogenation of phenylacetylene

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Science China Materials 2020年第6期63卷 982-992页

作者： Fu Yang Shipeng Ding Hongbing Songm Ning Yan Department of Chemical and Biomolecular Engineering National University of Singapore4 Engineering Drive 4117585Singapore School of Environmental and Chemical Engineering Jiangsu University of Science and TechnologyZhenjiang 212003China College of Chemical Engineering Qingdao University Science&TechnologyQingdao 266042China

Combining the advantages of both heterogeneous and homogeneous catalysts,single-atom catalysts(SACs)with unique electronic properties have shown excellent catalytic ***,we report single-atom Pd dispersed on nanoscale TiO2 prepared by self-assembly method as efficient and selective catalysts for the hydrogenation of phenylacetylene to *** catalysts were characterized by N2 adsorption/desorption,X-ray diffraction(XRD),transmission electron microscopy(TEM),X-ray photoelectron spectroscopy(XPS),diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)and X-ray absorption spectroscopy(XAS).0.2 Pd-TiO2(150℃)possessing dominant single-atom Pd species,exhibited a turnover frequency(TOF)of over 8000 h^-1 with 91%selectivity towards styrene at room *** increasing Pd loading from 0.2%to 0.5%and 1.5%resulted in the decrease of activity probably due to the formation of Pd ***,the 0.2 Pd-TiO2 prepared by self-assembly strategy showed better catalytic performance than commercial 10%Pd/C and0.2 Pd-TiO2 synthesized by using impregnation method.

关键词： single-atom catalyst palladium nanoscale T i02 semihydrogenation self-assembly method

Advances in Electrocatalytic Semi-Hydrogenation of Acetylene in Aqueous Electrolyte: Progress, Challenges, and Opportunities

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Renewables 2023年第3期1卷 278-293页

作者： Zihao Yan Libang Xu Huiyuan Zhu Department of Chemistry University of VirginiaCharlottesvilleVirginia 22904

Catalytic hydrogenation is a foundational pillar of the chemical ***,semi-hydrogenation of acetylene(C_(2)H_(2))to ethylene(C_(2)H_(4))is an important industrial reaction to generate polymer-grade C_(2)H_(4) from crude streams for polyethylene *** industrial C_(2)H_(2) semi-hydrogenation process is currently dominated by the thermocatalytic route that involves cost-prohibitive Pdbased catalysts,high operation temperature,and excess hydrogen *** semi-hydrogenation of C_(2)H_(2) is also hindered by limited C_(2)H_(4) selectivity due to unwanted ***,seeking strategies to improve the catalyst performance while reducing energy consumption and capital expenditure of the current hydrogenation schemes is essential to the petrochemical ***,recent advances in electrocatalytic C_(2)H_(2) semi-hydrogenation systems lead to a sustainable alternative to traditional thermocatalytic *** renewable electricity as an energy source and water as a hydrogen source,electrocatalytic systems can operate under ambient conditions with tunable selectivity toward C_(2)H_(4).In this review,we first discuss the reactor design for electrocatalytic C_(2)H_(2) *** then review the computational studies for understanding and predicting the catalytic behavior ofmetal *** also summarize advanced electrocatalysts categorized into Cu-based and non-Cu-based ***,we provide perspectives on the opportunities to overcome existing challenges for future practical application of electrocatalytic C_(2)H_(2) semihydrogenation.

关键词： acetylene ethylene electrocatalysis semihydrogenation