Electrocatalytic CO2 Reduction with a Ruthenium Catalyst in Solution and on Nanocrystalline TiO2

Li, Ting‐Ting; Shan, Bing; Xu, Wei; Meyer, Thomas J.

doi:10.1002/cssc.201900730

Title: Electrocatalytic CO₂ Reduction with a Ruthenium Catalyst in Solution and on Nanocrystalline TiO₂

Journal Article · Wed May 08 00:00:00 EDT 2019 · ChemSusChem

DOI:https://doi.org/10.1002/cssc.201900730· OSTI ID:1612323

^[1]; Shan, Bing ^[2]; Xu, Wei ^[1];

^[2]

Ningbo University (China)
Univ. of North Carolina, Chapel Hill, NC (United States)

Abstract A Ru ^II complex [Ru(PO ₃ Et ₂ ‐ph‐tpy)(6‐mbpy)(NCCH ₃ )] ²⁺ [PO ₃ Et ₂ ‐ph‐tpy=diethyl(4‐[(2,2′:6′,2′′‐terpyridin)‐4′‐yl]phenyl)phosphonate; 6‐mbpy=6‐methyl‐2,2′‐bipyridine] is explored as a molecular catalyst for electrocatalytic CO ₂ reduction in both a homogeneous solution and, as a phosphonated derivative, on nanocrystalline‐TiO ₂ surfaces. In CH ₃ CN, the complex acts as a selective electrocatalyst for reduction of CO ₂ to CO at a low overpotential of 340 mV but with a limited turnover number (TON). An enhancement in reactivity was observed by immobilizing the phosphonated derivative of the catalyst on a nanocrystalline‐TiO ₂ electrode surface, with the catalyst surface protected by a thin overlayer of NiO. The surface‐functionalized electrode was characterized by X‐ray photoelectron and diffuse reflectance spectroscopies (XPS and DRS). Electrocatalytic reduction of CO ₂ to CO occurred at −1.65 V versus Fc ^+/0 with a TON of 237 per catalyst site during 4 h of electrocatalysis. Post‐catalysis XPS measurements reveal that the molecular structure of the catalyst is retained on TiO ₂ after the long‐term electrocatalysis.

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Research Organization:: University of North Carolina, Chapel Hill, NC (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: SC0015739

OSTI ID:: 1612323

Alternate ID(s):: OSTI ID: 1512825

Journal Information:: ChemSusChem, Vol. 12, Issue 11; ISSN 1864-5631

Publisher:: ChemPubSoc EuropeCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 25 works

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Title: Electrocatalytic CO₂ Reduction with a Ruthenium Catalyst in Solution and on Nanocrystalline TiO₂