Chelating N-Heterocyclic Carbene Ligands Enable Tuning of Electrocatalytic CO2 Reduction to Formate and Carbon Monoxide: Surface Organometallic Chemistry

Cao, Zhi; Derrick, Jeffrey S.; Xu, Jun; Gao, Rui; Gong, Ming; Nichols, Eva M.; Smith, Peter T.; Liu, Xingwu; Wen, Xiaodong; Copéret, Christophe; Chang, Christopher J.

doi:10.1002/anie.201800367

Chelating N-Heterocyclic Carbene Ligands Enable Tuning of Electrocatalytic CO₂ Reduction to Formate and Carbon Monoxide: Surface Organometallic Chemistry

Journal Article · Thu Mar 01 00:00:00 EST 2018 · Angewandte Chemie (International Edition)

DOI:https://doi.org/10.1002/anie.201800367· OSTI ID:1480786

^[1]; Derrick, Jeffrey S. ^[2]; Xu, Jun ^[3]; Gao, Rui ^[4]; Gong, Ming ^[2]; Nichols, Eva M. ^[2]; Smith, Peter T. ^[2]; Liu, Xingwu ^[4]; Wen, Xiaodong ^[4]; Copéret, Christophe ^[3]; ^[2]

Univ. of California, Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
ETH Zurich, Zurich (Switzerland)
Chinese Academy of Sciences (CAS), Shanxi (China); Synfuels China, Beijing (China)

Reported here is the chelate effect as a design principle for tuning heterogeneous catalysts for electrochemical CO₂ reduction. Palladium functionalized with a chelating tris-N-heterocyclic carbene (NHC) ligand (Pd-timtmbMe) exhibits a 32-fold increase in activity for electrochemical reduction of CO₂ to C1 products with high Faradaic efficiency (FE_C1=86 %) compared to the parent unfunctionalized Pd foil (FE=23 %), and with sustained activity relative to a monodentate NHC-ligated Pd electrode (Pd-mimtmb^Me). Here, the results highlight the contributions of the chelate effect for tailoring and maintaining reactivity at molecular-materials interfaces enabled by surface organometallic chemistry.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1480786

Alternate ID(s):: OSTI ID: 1429150

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 18 Vol. 57; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Chelating N‐Heterocyclic Carbene Ligands Enable Tuning of Electrocatalytic CO ₂ Reduction to Formate and Carbon Monoxide: Surface Organometallic Chemistry

Journal Article · Thu Mar 22 20:00:00 EDT 2018 · Angewandte Chemie · OSTI ID:1429155

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
CO 2 reduction
N-heterocyclic carbenes
electrocatalysis
palladium
surface chemistry