Atomically Dispersed Ru-doped Ti4O7 Electrocatalysts for Chlorine Evolution Reaction with a Universal Activity

Lee, Woonghee; Choung, Seokhyun; Kim, Seok; Hong, Jiyun; Kim, Doyeon; Tarpeh, William A.; Han, Jeong Woo; Cho, Kangwoo

doi:10.1002/smll.202401248

Title: Atomically Dispersed Ru-doped Ti₄O₇ Electrocatalysts for Chlorine Evolution Reaction with a Universal Activity

Journal Article · 19 April 2024 · Small

DOI: https://doi.org/10.1002/smll.202401248 · OSTI ID:2403666

^[1]; Choung, Seokhyun ^[2]; Kim, Seok ^[3]; Hong, Jiyun ^[4]; Kim, Doyeon ^[5]; Tarpeh, William A. ^[6]; Han, Jeong Woo ^[2];

^[7]

Stanford Univ., CA (United States); Pohang Univ. of Science and Technology (POSTECH) (Korea, Republic of); SLAC
Seoul National Univ. (Korea, Republic of)
Pohang Univ. of Science and Technology (POSTECH) (Korea, Republic of); Swiss Federal Institute of Aquatic Science and Technology (Eawag), Dübendorf (Switzerland)
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Pohang Univ. of Science and Technology (POSTECH) (Korea, Republic of)
Stanford Univ., CA (United States)
Pohang Univ. of Science and Technology (POSTECH) (Korea, Republic of); Yonsei Univ. International Campus, Incheon (Korea, Republic of)

Chlorine has been supplied by the chlor-alkali process that deploys dimensionally stable anodes (DSAs) for the electrochemical chlorine evolution reaction (ClER). The paramount bottlenecks have been ascribed to an intensive usage of precious elements and inevitable competition with the oxygen evolution reaction. Herein, a unique case of Ru²⁺-O₄ active motifs anchored on Magnéli Ti₄O₇ (Ru-Ti₄O₇) via a straightforward wet impregnation and mild annealing is reported. The Ru-Ti₄O₇ performs radically active ClER with minimal deployment of Ru (0.13 wt%), both in 5 m NaCl (pH 2.3) and 0.1 $$\tiny{M}$$ NaCl (pH 6.5) electrolytes. Scanning electrochemical microscopy demonstrates superior ClER selectivity on Ru-Ti₄O₇ compared to the DSA. Operando X-ray absorption spectroscopy and density functional theory calculations reveal a universally active ClER (over a wide range of pH and [Cl^-]), through a direct adsorption of Cl^- on Ru²⁺-O₄ sites as the most plausible pathway, together with stabilized ClO* at low [Cl^-] and high pH.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC); National Research Foundation of Korea (NRF)

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 2403666

Journal Information:: Small, Journal Name: Small Journal Issue: 35 Vol. 20; ISSN 1613-6810

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Magnéli Ti4O7
chlorine evolution reaction
electrocatalysis
scanning electrochemical microscopy
single-atom catalysts

Title: Atomically Dispersed Ru-doped Ti4O7 Electrocatalysts for Chlorine Evolution Reaction with a Universal Activity

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References (52)

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Title: Atomically Dispersed Ru-doped Ti₄O₇ Electrocatalysts for Chlorine Evolution Reaction with a Universal Activity