Noninnocent Proton-Responsive Ligand Facilitates Reductive Deprotonation and Hinders CO2 Reduction Catalysis in [Ru(tpy)(6DHBP)(NCCH3 )]2+ (6DHBP = 6,6'-(OH)2 bpy)

Duan, Lele; Manbeck, Gerald F.; Kowalczyk, Marta; Szalda, David J.; Muckerman, James T.; Himeda, Yuichiro; Fujita, Etsuko

doi:10.1021/acs.inorgchem.6b00398

Title: Noninnocent Proton-Responsive Ligand Facilitates Reductive Deprotonation and Hinders CO₂ Reduction Catalysis in [Ru(tpy)(6DHBP)(NCCH₃ )]²⁺ (6DHBP = 6,6'-(OH)₂ bpy)

Journal Article · Thu Apr 14 00:00:00 EDT 2016 · Inorganic Chemistry

DOI:https://doi.org/10.1021/acs.inorgchem.6b00398· OSTI ID:1335424

Duan, Lele ^[1]; Manbeck, Gerald F. ^[1]; Kowalczyk, Marta ^[1]; Szalda, David J. ^[2]; Muckerman, James T. ^[1]; Himeda, Yuichiro ^[3]; Fujita, Etsuko ^[1]

Brookhaven National Lab. (BNL), Upton, NY (United States). Dept. of Chemistry
Brookhaven National Lab. (BNL), Upton, NY (United States). Dept. of Chemistry; Baruch College, New York, NY (United States). Department of Natural Science
National Inst. of Advanced Industrial Science and Technology (AIST), Tsukuba (Japan)

Ruthenium complexes with proton-responsive ligands [Ru(tpy)(nDHBP)(NCCH₃)](CF₃SO₃)₂ (tpy = 2,2':6',2"-terpyridine; nDHBP = n,n'-dihydroxy-2,2'-bipyridine, n = 4 or 6) were examined in this study for reductive chemistry and as catalysts for CO₂ reduction. Electrochemical reduction of [Ru(tpy)(nDHBP)(NCCH₃)]²⁺ generates deprotonated species through interligand electron transfer in which the initially formed tpy radical anion reacts with a proton source to produce singly and doubly deprotonated complexes that are identical to those obtained by base titration. A third reduction (i.e., reduction of [Ru(tpy)(nDHBP–2H⁺)]⁰) triggers catalysis of CO₂ reduction; however, the catalytic efficiency is strikingly lower than that of unsubstituted [Ru(tpy)(bpy)(NCCH₃)]²⁺ (bpy = 2,2'-bipyridine). Cyclic voltammetry, bulk electrolysis, and spectroelectrochemical infrared experiments suggest the reactivity of CO₂ at both the Ru center and the deprotonated quinone-type ligand. Lastly, the Ru carbonyl formed by the intermediacy of a metallocarboxylic acid is stable against reduction, and mass spectrometry analysis of this product indicates the presence of two carbonates formed by the reaction of DHBP–2H⁺ with CO₂.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

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

Grant/Contract Number:: SC00112704

OSTI ID:: 1335424

Report Number(s):: BNL-112052-2016-JA; R&D Project: CO026; KC0304030

Journal Information:: Inorganic Chemistry, Vol. 55, Issue 9; ISSN 0020-1669

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 30 works

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Nickel( ii ) pincer complexes demonstrate that the remote substituent controls catalytic carbon dioxide reduction Burks, Dalton B.; Davis, Shakeyia; Lamb, Robert W. Chemical Communications, Vol. 54, Issue 31 https://doi.org/10.1039/c7cc09507d	journal	January 2018
Effect of PDI ligand binding pattern on the electrocatalytic activity of two Ru(II) complexes for CO ₂ reduction Shi, Ning‐ning; Xie, Wang‐jing; Gao, Wei‐song Applied Organometallic Chemistry, Vol. 34, Issue 4 https://doi.org/10.1002/aoc.5551	journal	February 2020
Molecular Catalysts with Intramolecular Re–O Bond for Electrochemical Reduction of Carbon Dioxide Rotundo, Laura; Polyansky, Dmitry E.; Gobetto, Roberto Inorganic Chemistry, Vol. 59, Issue 17 https://doi.org/10.1021/acs.inorgchem.0c01181	journal	August 2020

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

CCDC 1478549: Experimental Crystal Structure Determination: ILEXAA : aqua-(2,2'-bipyridine-6,6'-diol)-(2,2':6',2''-terpyridine)-ruthenium(ii) perchlorate trifluoromethanesulfonate monohydrate Duan, Lele; Manbeck, Gerald F.; Kowalczyk, Marta https://doi.org/10.5517/ccdc.csd.cc1lmk4x The current record is supplemented by this dataset	dataset	May 2016
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Title: Noninnocent Proton-Responsive Ligand Facilitates Reductive Deprotonation and Hinders CO2 Reduction Catalysis in [Ru(tpy)(6DHBP)(NCCH3 )]2+ (6DHBP = 6,6'-(OH)2 bpy)

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