Well-Defined Rhodium–Gallium Catalytic Sites in a Metal–Organic Framework: Promoter-Controlled Selectivity in Alkyne Semihydrogenation to E-Alkenes [Well-Defined Rh–Ga Catalytic Sites in a Metal–Organic Framework: Promoter-Controlled Selectivity in Alkyne Semihydrogenation to E-Alkenes]

Desai, Sai Puneet; Ye, Jingyun; Zheng, Jian; Ferrandon, Magali S.; Webber, Thomas E.; Platero-Prats, Ana E.; Duan, Jiaxin; Garcia-Holley, Paula; Camaioni, Donald M.; Chapman, Karena W.; Delferro, Massimiliano; Farha, Omar K.; Fulton, John L.; Gagliardi, Laura; Lercher, Johannes A.; Penn, R. Lee; Stein, Andreas; Lu, Connie C.

doi:10.1021/jacs.8b08550

Well-Defined Rhodium–Gallium Catalytic Sites in a Metal–Organic Framework: Promoter-Controlled Selectivity in Alkyne Semihydrogenation to E-Alkenes [Well-Defined Rh–Ga Catalytic Sites in a Metal–Organic Framework: Promoter-Controlled Selectivity in Alkyne Semihydrogenation to E-Alkenes]

Journal Article · Tue Oct 23 00:00:00 EDT 2018 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.8b08550· OSTI ID:1484223

Desai, Sai Puneet ^[1]; ^[1]; ^[2]; Ferrandon, Magali S. ^[3]; ^[1]; ^[4]; Duan, Jiaxin ^[1]; Garcia-Holley, Paula ^[5]; ^[2]; ^[6]; ^[3]; ^[5]; ^[2]; ^[1]; Lercher, Johannes A. ^[7]; ^[1]; ^[1]; ^[1]

Univ. of Minnesota, Minneapolis, MN (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)
Univ. Autonoma de Madrid, Madrid (Spain); Argonne National Lab. (ANL), Argonne, IL (United States)
Northwestern Univ., Evanston, IL (United States)
Argonne National Lab. (ANL), Argonne, IL (United States); Stony Brook Univ., Stony Brook, NY (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Technische Univ. Munchen, Garching (Germany)

Promoters are ubiquitous in industrial heterogeneous catalysts. The wider roles of promoters in accelerating catalysis and/or controlling selectivity are, however, not well understood. A model system has been developed where a heterobimetallic active site comprising an active metal (Rh) and a promoter ion (Ga) are preassembled and delivered onto a metal-organic framework (MOF) support, NU-1000. The Rh-Ga sites in NU-1000 selectively catalyze the hydrogenation of acyclic alkynes to E-alkenes. The overall stereoselectivity is complementary to the well-known Lindlar’s catalyst, which generates Zalkenes. In conclusion, the role of the Ga in promoting this unusual selectivity is evidenced by the lack of semihydrogenation selectivity when Ga is absent and only Rh is present in the active site.

View Accepted Manuscript (DOE)

Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Energy Frontier Research Center for Inorganometallic Catalyst Design (ICDC); Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1484223

Alternate ID(s):: OSTI ID: 1507435

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 45 Vol. 140; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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