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Tuning catalytic properties using an atomically dispersed metal overlayer on transition metal carbide substrates

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National Science Review 2017年第6期4卷 788-789页

作者： jingguang g.chen Chemistry Department Brookhaven National Laboratory Department of Chemical Engineering Columbia University

Aqueous-phase reforming of methanol(APRM)represents an important reaction to produce hydrogen for lowtemperature polymer electrode membrane(PEM)hydrogen fuel *** ideal catalyst for APRM should show high activity towar... 详细信息

关键词： PgM TMC Tuning catalytic properties using an atomically dispersed metal overlayer on transition metal carbide substrates Pt

Challenges and opportunities in plasma-activated reactions of CO_(2) with light alkanes

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Journal of Energy Chemistry 2023年第9期84卷 424-427页

作者： Lea R.Winter jingguang g.chen Department of Chemical and Environmental Engineering Yale UniversityNew HavenCT 06520United States Department of Chemical Engineering Columbia UniversityNew YorkNY 10027United States Chemistry Division Brookhaven National LaboratoryUptonNY 11973United States

Mitigation of the deleterious environmental impacts associated with CO_(2) emissions requires the development of more sustainable processes for synthesizing fuels and *** conversion of abundant yet difficult to activate molecules such as CO_(2) and surplus light alkanes from shale gas to desirable products can potentially reduce reliance upon conventional fossil-based ***,co-conversion of CO_(2) with abundant light alkanes such as methane and ethane using atmospheric-pressure.

关键词： alkanes methane synthesizing

Reduction-induced metal/oxide interfacial sites for selective CO_(2) hydrogenation

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SmartMat 2023年第4期4卷 199-209页

作者： Zhenhua Xie Sooyeon Hwang jingguang g.chen Department of Chemical Engineering Columbia UniversityNew YorkNew YorkUSA Chemistry Division Brookhaven National LaboratoryUptonNew YorkUSA Center for Functional Nanomaterials Brookhaven National LaboratoryUptonNew YorkUSA

The interfacial structures of bimetallic-derived catalysts play an important role in promoting the activation of reactants such as CO_(2).In particular,both the physical property(e.g.,local bonding environment)and the electronic property(e.g.,oxidation state)can evolve from their native states under different environments,such as upon reduction and during the catalytic ***,taking the CO_(2) hydrogenation reaction over Rh-based catalysts as a case study,the present work compares the interfacial structures in tuning the selectivity toward CH_(4) or *** combination of ex situ and in situ characterization reveals two representative interfacial structures:the Rh/CeO_(x) interface formed over Rh/CeO_(2) is active and selective to produce CH_(4)(~95%)by following a formate-mediated pathway;in comparison,the InO_(x)/Rh interface derived after reduction is active for CO_(2) activation and enables a redox mechanism for the exclusive formation of CO(~100%).This work provides insights into the environment-induced structural evolution at the metal−oxide interfaces,as well as the role of distinct interfacial active sites in tuning the selectivity of CO_(2) hydrogenation.

关键词： CO_(2) hydrogenation interfacial structure Rh-based catalysts structural evolution

Coupling CO_(2)reduction with ethane aromatization for enhancing catalytic stability of iron-modified ZSM-5

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Journal of Energy Chemistry 2022年第3期31卷 210-217,I0007页

作者： Zhenhua Xie Elaine gomez Dong Wang Ji Hoon Lee Tiefeng Wang jingguang g.chen Department of Chemical Engineering Columbia UniversityNew YorkNY 10027USA Chemistry Division Brookhaven National LaboratoryUptonNY 11973USA Department of Chemical Engineering Tsinghua UniversityBeijing100084 BeijingChina

The shale gas revolution and the carbon-neutrality goal are motivating the landscape toward the synthesis of value-added chemicals or fuels from underutilized ethane with the assistance of greenhouse gas CO_(2).Combining ethane aromatization with CO_(2)reduction offers an opportunity to directly produce liquid products for facile separation,storage,and *** the present work,Fe/ZSM-5 catalysts showed promise in the simultaneous CO_(2)reduction and ethane aromatization at atmospheric pressure and 873 *** catalysts were further investigated using X-ray diffraction(XRD)and X-ray absorption fine structure(XAFS)measurements under in-situ conditions,indicating that most of Fe species existed in the form of Fe oxides and a portion of Fe was incorporated into the ZSM-5 framework generating Lewis acid *** types of Fe species remained almost unchanged under reaction conditions,contributing to an enhanced aromatization activity of Fe/*** effects of CO_(2)and steam on the acid sites and in turn aromatization activity were also investigated by transient studies,which exhibited a reversible modification ***,CO_(2)was identified to be critical to enhance coke resistance and in turn catalyst *** work highlights the feasibility of using CO_(2)to assist the upgrading of abundant ethane from shale gas to aromatics over non-precious Fe-based zeolite catalysts.

关键词： Ethane CO_(2) Aromatization Fe-modified ZSM-5

Utilizing bimetallic catalysts to mitigate coke formation in dry reforming of methane

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Journal of Energy Chemistry 2022年第5期31卷 124-142页

作者： Jaylin Sasson Bitters Tina He Elizabeth Nestler Sanjaya D.Senanayake jingguang g.chen cheng Zhang College of Liberal Arts and Sciences Long Island University(Post)BrookvilleNY 11548United States Department of Molecular Biosciences University of Texas at AustinAustinTX 78712United States Chemistry Division Brookhaven National LaboratoryUptonNY 11973United States Department of Chemical Engineering Columbia UniversityNew YorkNY 10027United States

Dry reforming of methane(DRM) involves the conversion of carbon dioxide(CO_(2)) and methane(CH_(4)) into syngas(a mixture of hydrogen, H_(2), and carbon monoxide, CO), which can then be used to produce a wide range of products by means of Fischer–Tropsch synthesis. DRM has gained much attention as a means of mitigating damage from anthropogenic greenhouse gas(gHgs) emissions to the environment and instead utilizing these gases as precursors for value-added chemicals or to synthesize sustainable fuels and chemicals. Carbon deposition or coke formation, a primary cause of catalyst deactivation, has proven to be a major challenge in the development of DRM catalysts. The use of nickel-and cobalt-based catalysts has been extensively explored for DRM for their high activity and low cost but suffer from poor stability due to coke formation that has hindered their commercialization. Numerous articles have reviewed the various aspects of catalyst deactivation and strategies for mitigation, but few has focused on the benefit of bimetallic catalysts for mitigating coke formation. Bimetallic catalysts, often improve the catalytic stability over their monometallic counterparts due to synergistic effects resulting from two metal-tometal interactions. This review will cover DRM literature for various bimetallic catalyst systems, including the effect of supports and promoters, on the mitigation of carbonaceous deactivation.

关键词： Dry reforming of methane Carbon dioxide Bimetallic catalysts Coke formation Catalyst stability

Synthesis and electrocatalytic applications of flower-like motifs and associated composites of nitrogen-enriched tungsten nitride(W2N3)

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Nano Research 2020年第5期13卷 1434-1443页

作者： Sha Tan Brian M.Tackett Qun He Ji Hoon Lee jingguang g.chen Stanislaus S.Wong Department of Chemistry State University of New York at Stony BrookStony BrookNY 11794-3400USA Department of Chemical Engineering Columbia UniversityNew YorkNY 10027USA Chemistry Department Building 555Brookhaven National LaboratoryUptonNY 11973USA

We have sought to improve the electrocatalytic performance of tungsten nitride through synthetic control over chemical composition and *** particular,we have generated a thermodynamically unstable but catalytically promising nitrogen-rich phase of tungsten via a hydrothermal generation of a tungsten oxide intermediate and subsequent annealing in *** net product consisted of three-dimensional(3D)micron-scale flower-like motifs of W2N3;this architecture not only evinced high structural stability but also incorporated the favorable properties of constituent two-dimensional *** a performance perspective,as-prepared 3D W2N3 demonstrated promising hydrogen evolution reaction(HER)activities,especially in an acidic environment with a measured overpotential value of−101 mV at a current density of 10 mA/cm^*** further enhance the electrocatalytic activity,small amounts of precious metal nanoparticles(such as Pt and Au),consisting of variable sizes,were uniformly deposited onto the underlying 3D W2N3 motifs using a facile direct deposition method;these composites were applied towards the CO2 reduction reaction(CO2RR).A highlight of this series of experiments was that Au/W2N3 composites were found to be a much more active HER(as opposed to either a CO2RR or a methanol oxidation reaction(MOR))catalyst.

关键词： tungsten nitride synthesis composite morphology control electrocatalysis

glycerol Electrooxidation over Precision-Synthesized gold Nanocrystals with Different Surface Facets

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Precision Chemistry 2024年第3期2卷 103-111页

作者： Hansen Mou Fang Lu Zechao Zhuang Qiaowan Chang Lihua Zhang Xiaobo chen Yugang Zhang jingguang g.chen Department of Chemical Engineering Columbia UniversityNew YorkNew York 10027United States School of Chemical Engineering and Bioengineering Washington State UniversityPullmanWashington 99164United States Center for Functional Nanomaterials Brookhaven National LaboratoryUptonNew York 11973United States Materials Science and Engineering Program State University of New York at BinghamtonBinghamtonNew York 13902United States Chemistry Division Brookhaven National LaboratoryUptonNew York 11973United States

Electrochemical glycerol oxidation(EgO)emerges as a promising route to valorize glycerol,an underutilized byproduct from biodiesel production,into value-added *** study employed three types of gold(Au)nanocrystals with controlled shapes to elucidate the facet-dependent electrocatalytic behavior in ***,rhombic dodecahedral,and cubic Au nanocrystals with{111},{110},and{100}facets,respectively,were precisely synthesized with uniform size and *** dodecahedra exhibited the lowest onset potential for EgO due to facile AuOH formation,while octahedra showed enhanced electrochemical activity for glycerol oxidation and resistance to ***-situ FTIR analysis revealed that Au{111}surfaces selectively favored C_(2) products,whereas Au{100}surfaces promoted C_(3) product formation,highlighting the significant effect of facet orientation on EgO performance and informing catalyst design.

关键词： Electrochemical glycerol oxidation Precision synthesis Shaped nanocrystals Au nanocrystals SAXS In-situ FTIR

Investigation of the role of Ca(OH)2 in the catalytic Alkaline Thermal Treatment of cellulose to produce H2 with integrated carbon capture

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Journal of Energy Chemistry 2017年第5期26卷 984-1000页

作者： Maxim R.Stonor Nicholas Ouassil jingguang g.chen Ah-Hyung Alissa Park Department of Chemical Engineering Columbia UniversityNYUSA Department of Earth and Environmental Engineering Columbia UniversityNYUSA Lenfest Center for Sustainable Energy Columbia UniversityNYUSA

The Alkaline Thermal Treatment(ATT)of biomass is one of the few biomass conversion processes that has a potential for BECCS(bio-energy with carbon capture and storage).Combining in-situ carbon capture withcreates a carbon-neutral process that has the potential to be *** study has shown that the conversion of cellulose tosuppressedcan be achieved through the reforming of gaseous intermediates in a fixed bed of 10%Ni/*** occurs at low temperatures≤773 K,which could allow for improved sustainability.

关键词： Hydrogen Biomass Alkaline Thermal Treatment Calcium hydroxide Calcium carbonate Carbon capture utilization storage Nickel Heterogeneous catalysis Catalytic reforming

选择氧化物载体调变乙醇重整和1,3-丁二烯加氢反应双金属催化剂(英文)

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催化学报 2013年第11期34卷 2009-2017页

作者：王铁峰 William Lonergan 陈经广清华大学化工系绿色反应工程与工艺北京市重点实验室北京100084 特拉华大学化学与生物分子工程系催化科技中心美国纽瓦克DE19716 哥伦比亚大学化工系美国纽约NY10027

研究了不同载体负载的Pt-Ni双金属和单金属催化剂上乙醇重整和1,3-丁二烯加氢反应性能, 以考察氧化物载体对双金属结构和催化活性的影响. 所用的氧化物载体包括γ-Al2O3, SiO2, TiO2, CeO2以及高比表面积(HSA)和低比表面积(LSA)ZrO2. ... 详细信息

研究了不同载体负载的Pt-Ni双金属和单金属催化剂上乙醇重整和1,3-丁二烯加氢反应性能, 以考察氧化物载体对双金属结构和催化活性的影响. 所用的氧化物载体包括γ-Al2O3, SiO2, TiO2, CeO2以及高比表面积(HSA)和低比表面积(LSA)ZrO2. 采用共浸渍法制备催化剂, 用CO化学吸附、透射电镜和扩展X射线吸收精细结构光谱进行催化剂表征, 采用傅里叶变换红外间歇反应器进行化学反应评价. 对于乙醇重整反应, Pt-Ni双金属催化剂优于单金属催化剂, Pt-Ni双金属催化剂活性顺序为TiO2>SiO2>-Al2O3≈LSA-ZrO2>CeO2>HSA-ZrO2. 对于1,3-丁二烯加氢反应, 在SiO2,TiO2和HSA-ZrO2载体上双金属催化剂优于单金属催化剂, Pt-Ni双金属催化剂活性顺序为SiO2>CeO2>-Al2O3>LSA-ZrO2>HSA-ZrO2≈TiO2.

关键词：铂镍双金属催化剂载体影响乙醇重整 1,3-丁二烯加氢扩展X射线吸收精细结构光谱