Enhanced Activity of Heterogeneous Pd(II) Catalysts on Acid-Functionalized Metal–Organic Frameworks

Otake, Ken-ichi; Ye, Jingyun; Mandal, Mukunda; Islamoglu, Timur; Buru, Cassandra T.; Hupp, Joseph T.; Delferro, Massimiliano; Truhlar, Donald G.; Cramer, Christopher J.; Farha, Omar K.

doi:10.1021/acscatal.9b01043

Title: Enhanced Activity of Heterogeneous Pd(II) Catalysts on Acid-Functionalized Metal–Organic Frameworks

Journal Article · Mon Apr 29 00:00:00 EDT 2019 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.9b01043· OSTI ID:1526641

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Northwestern Univ., Evanston, IL (United States); Kyoto Univ., Kyoto (Japan)
Univ. of Minnesota, Minneapolis, MN (United States)
Northwestern Univ., Evanston, IL (United States)
Argonne National Lab. (ANL), Lemont, IL (United States)

Single-site heterogeneous catalysts (SSHCs) play important roles in fundamental science and technology, owing to the molecular level control of structure–support interactions that is possible in these systems. Recently, SSHCs supported by acidic oxides have attracted particular interest because catalytically active metal centers can be formed at the surface sites. Here, we incorporated a palladium SSHC in phosphated and sulfated metal–organic frameworks (MOFs), hafnium-based MOF-808 (Hf-MOF-808-PO₄ and Hf-MOF-808-SO₄). The structural and electronic properties of the Pd(II) sites coordinated to the acidic sites in these MOFs were investigated through X-ray photoelectron spectroscopy, vibrational spectroscopy, X-ray crystallographic techniques, catalytic studies, and quantum mechanical electronic structure calculations employing density functional theory. We demonstrated that the presence of node-bound acidic functional groups stabilizes the Pd(II) site in these MOFs, resulting in enhanced catalytic activities (compared to in the nonacid functionalized Hf-MOF-808) in the oxidative Heck reaction where Pd(II) is the active species. The density functional calculations support the interpretation that the acid functionalization of the MOF node can stabilize the Pd(0) intermediate state during the catalytic reactions, thereby suppressing Pd(0) aggregation leading to catalyst deactivation. Furthermore, these findings offer insights and methodology for the catalytic investigation of SSHCs in MOFs.

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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)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1526641

Journal Information:: ACS Catalysis, Vol. 9, Issue 6; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 59 works

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
metal−organic frameworks
single-site heterogeneous catalyst
oxidative Heck reaction
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CCDC 1901984: Experimental Crystal Structure Determination Ken-ichi, Otake,; Jingyun, Ye,; Mukunda, Mandal, https://doi.org/10.5517/ccdc.csd.cc21v5bf The current record is supplemented by this dataset	dataset	January 2021
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CCDC 1901986: Experimental Crystal Structure Determination Ken-ichi, Otake,; Jingyun, Ye,; Mukunda, Mandal, https://doi.org/10.5517/ccdc.csd.cc21v5dh The current record is supplemented by this dataset	dataset	January 2021
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