EAGER:GOALI: Bulk Intermetallics with well-defined active sites for selectivity control in selective hydrogenations

EAGER:GOALI：具有明确活性位点的块状金属间化合物，用于选择性加氢中的选择性控制

基本信息

批准号：
1748365
负责人：
Robert Rioux
金额：
$ 20.64万
依托单位：
Pennsylvania State Univ University Park
依托单位国家：
美国
项目类别：
Standard Grant
财政年份：
2017
资助国家：
美国
起止时间：
2017-10-01 至 2020-09-30
项目状态：
已结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=1748365&HistoricalAwards=false
关键词：
EAGER GOALI Bulk Intermetallics well

项目摘要

This research project investigates a new class of heterogeneous catalysts for the selective hydrogenation reactions of light hydrocarbons to higher-value chemical intermediates of value to the petrochemical industry. Selectivity refers to the ability of a catalyst to favor one product over another when multiple products are possible. As such, it is possible to control selectivity by changing the surface composition of a catalyst. This research project investigates a class of inorganic solids, intermetallic compounds, that have ordered assemblies of small metal clusters of various size and composition. These intermetallic compounds have potential as highly selective catalysts for important hydrocarbon hydrogenation reactions. Computational studies and experiment studies are being combined to identify catalyst compositions that display both high catalytic activity and high selectivity toward the desired products. Crystallographically well-defined intermetallic compounds are being utilized to understand the impact of catalytically-active metal atom nuclearity on catalytic selectivity. Intermetallic compounds are being synthesized with varying compositions across the gamma-brass phase to control both nuclearity and the number of clusters. Intermetallics of the form M-Zn (M = Pd, Cu and Ag) have been carefully chosen since they contain contiguous cluster sizes of catalytic metal from monomers to hexamers. M-Zn bulk intermetallics are being examined for partial hydrogenation reactions of mixed feedstocks (alkyne plus alkene and alkene plus aromatic). The results will demonstrate the impact of cluster size on catalyst selectivity. The results can be used to identify selective cluster sizes for hydrogenation that will then become targets for synthesis in a high surface area nanoparticle form. The study is being conducted in collaboration with an industrial partner (ExxonMobil) who provides access to synchrotron-based X-ray absorption catalyst characterization tools, while also delivering industrially-relevant guidance to the graduate students involved in the project.

该研究项目研究一类新型多相催化剂，用于轻质烃的选择性加氢反应，生成对石化工业有价值的高价值化学中间体。选择性是指当可能有多种产物时，催化剂有利于一种产物而不是另一种产物的能力。因此，可以通过改变催化剂的表面组成来控制选择性。该研究项目研究了一类无机固体，即金属间化合物，它们具有不同尺寸和成分的小金属簇的有序组装体。这些金属间化合物具有作为重要烃加氢反应的高选择性催化剂的潜力。计算研究和实验研究相结合，以确定对所需产物表现出高催化活性和高选择性的催化剂组合物。晶体学上明确的金属间化合物被用来了解催化活性金属原子核对催化选择性的影响。人们正在合成具有不同成分的γ-黄铜相金属间化合物，以控制核性和簇数。 M-Zn（M = Pd、Cu 和 Ag）形式的金属间化合物经过精心挑选，因为它们含有从单体到六聚体的连续簇尺寸的催化金属。 M-Zn 块状金属间化合物正在研究混合原料（炔烃加烯烃和烯烃加芳烃）的部分加氢反应。结果将证明簇尺寸对催化剂选择性的影响。结果可用于确定用于氢化的选择性簇尺寸，然后该簇尺寸将成为高表面积纳米颗粒形式合成的目标。该研究是与工业合作伙伴（埃克森美孚）合作进行的，该合作伙伴提供基于同步加速器的 X 射线吸收催化剂表征工具，同时还为参与该项目的研究生提供工业相关指导。

项目成果

期刊论文数量（4）

专著数量（0）

科研奖励数量（0）

会议论文数量（0）

专利数量（0）

Generalized approach for the synthesis of silica supported Pd-Zn, Cu-Zn and Ni-Zn gamma brass phase nanoparticles

DOI：
10.1016/j.cattod.2018.10.050
发表时间：
2019-08-15
期刊：
CATALYSIS TODAY
影响因子：
5.3
作者：
Dasgupta, Anish;Zimmerer, Eric K.;Rioux, Robert M.
通讯作者：
Rioux, Robert M.

Enhancement of Alkyne Semi-Hydrogenation Selectivity by Electronic Modification of Platinum

DOI：
10.1021/acscatal.9b04070
发表时间：
2020-05
期刊：
ACS Catalysis
影响因子：
12.9
作者：
Zhenshu Wang;Aaron Garg;Linxi Wang;Haoran He;Anish Dasgupta;D. Zanchet;M. Janik;R. Rioux;
通讯作者：
Zhenshu Wang;Aaron Garg;Linxi Wang;Haoran He;Anish Dasgupta;D. Zanchet;M. Janik;R. Rioux;

Competitive Hydrogenation between Linear Alkenes and Aromatics on Close-Packed Late Transition Metal Surfaces