Sintering-Resistant Single-Site Nickel Catalyst Supported by Metal–Organic Framework
- Northwestern Univ., Evanston, IL (United States)
- Univ. of Minnesota, Minneapolis, MN (United States)
- Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
- Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Purdue Univ., West Lafayette, IN (United States)
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Inst. for Integrated Catalysis
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Inst. for Integrated Catalysis; Technische Univ. Munchen, Garching (Germany)
- Northwestern Univ., Evanston, IL (United States); King Abdulaziz Univ., Jeddah (Saudi Arabia)
Developing supported single-site catalysts is an important goal in heterogeneous catalysis since the welldefined active sites afford opportunities for detailed mechanistic studies, thereby facilitating the design of improved catalysts. We present in this paper a method for installing Ni ions uniformly and precisely on the node of a Zr-based metal–organic framework (MOF), NU-1000, in high density and large quantity (denoted as Ni-AIM) using atomic layer deposition (ALD) in a MOF (AIM). Ni-AIM is demonstrated to be an efficient gas-phase hydrogenation catalyst upon activation. The structure of the active sites in Ni-AIM is proposed, revealing its single-site nature. More importantly, due to the organic linker used to construct the MOF support, the Ni ions stay isolated throughout the hydrogenation catalysis, in accord with its long-term stability. A quantum chemical characterization of the catalyst and the catalytic process complements the experimental results. With validation of computational modeling protocols, we further targeted ethylene oligomerization catalysis by Ni-AIM guided by theoretical prediction. Given the generality of the AIM methodology, this emerging class of materials should prove ripe for the discovery of new catalysts for the transformation of volatile substrates.
- Research Organization:
- Energy Frontier Research Centers (EFRC) (United States). Energy Frontier Research Center for Inorganometallic Catalyst Design (ICDC); Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
- Sponsoring Organization:
- USDOD; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; National Science Foundation (NSF); International Institute for Nanotechnology (IIN); State of Illinois; National Institutes of Health (NIH)
- Grant/Contract Number:
- SC0012702; AC02-06CH11357
- OSTI ID:
- 1387404
- Journal Information:
- Journal of the American Chemical Society, Vol. 138, Issue 6; Related Information: ICDC partners with University of Minnesota(lead); Argonne National Laboratory; Clemson University; Dow Chemical Company; Northwestern University; Pacific Northwest National Laboratory; University of California Davis; University of Washington; ISSN 0002-7863
- Publisher:
- American Chemical Society (ACS)Copyright Statement
- Country of Publication:
- United States
- Language:
- English
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