Sintering-Resistant Single-Site Nickel Catalyst Supported by Metal–Organic Framework

Li, Zhanyong; Schweitzer, Neil M.; League, Aaron B.; Bernales, Varinia; Peters, Aaron W.; Getsoian, Andrew “Bean”; Wang, Timothy C.; Miller, Jeffrey T.; Vjunov, Aleksei; Fulton, John L.; Lercher, Johannes A.; Cramer, Christopher J.; Gagliardi, Laura; Hupp, Joseph T.; Farha, Omar K.

doi:10.1021/jacs.5b12515

Sintering-Resistant Single-Site Nickel Catalyst Supported by Metal–Organic Framework

Journal Article · Tue Feb 02 04:00:00 EST 2016 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.5b12515· OSTI ID:1387404

Li, Zhanyong ^[1]; Schweitzer, Neil M. ^[1]; League, Aaron B. ^[2]; Bernales, Varinia ^[2]; Peters, Aaron W. ^[1]; Getsoian, Andrew “Bean” ^[3]; Wang, Timothy C. ^[1]; Miller, Jeffrey T. ^[4]; Vjunov, Aleksei ^[5]; Fulton, John L. ^[5]; Lercher, Johannes A. ^[6]; Cramer, Christopher J. ^[2]; Gagliardi, Laura ^[2]; Hupp, Joseph T. ^[1]; Farha, Omar K. ^[7]

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.

View Accepted Manuscript (DOE)

Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Inorganometallic Catalyst Design Center (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

Alternate ID(s):: OSTI ID: 1255383

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 6 Vol. 138; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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