Electrochemical trapping of metastable Mn3+ ions for activation of MnO2 oxygen evolution catalysts

Chan, Zamyla Morgan; Kitchaev, Daniil A.; Weker, Johanna Nelson; Schnedermann, Christoph; Lim, Kipil; Ceder, Gerbrand; Tumas, William; Toney, Michael F.; Nocera, Daniel G.

doi:10.1073/pnas.1722235115

Title: Electrochemical trapping of metastable Mn³⁺ ions for activation of MnO₂ oxygen evolution catalysts

Journal Article · 21 May 2018 · Proceedings of the National Academy of Sciences of the United States of America

DOI: https://doi.org/10.1073/pnas.1722235115 · OSTI ID:1438083

Chan, Zamyla Morgan ^[1]; Kitchaev, Daniil A. ^[2]; Weker, Johanna Nelson ^[3]; Schnedermann, Christoph ^[1]; Lim, Kipil ^[4]; Ceder, Gerbrand ^[5]; Tumas, William ^[6]; Toney, Michael F. ^[3];

^[1]

Harvard Univ., Cambridge, MA (United States)
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., Menlo Park, CA (United States)
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
National Renewable Energy Lab. (NREL), Golden, CO (United States)

Electrodeposited manganese oxide films are promising catalysts for promoting the oxygen evolution reaction (OER), especially in acidic solutions. The activity of these catalysts is known to be enhanced by the introduction of Mn³⁺. We present in situ electrochemical and X-ray absorption spectroscopic studies, which reveal that Mn³⁺ may be introduced into MnO₂ by an electrochemically induced comproportionation reaction with Mn²⁺ and that Mn³⁺ persists in OER active films. Extended X-ray absorption fine structure (EXAFS) spectra of the Mn³⁺-activated films indicate a decrease in the Mn–O coordination number, and Raman microspectroscopy reveals the presence of distorted Mn–O environments. Computational studies show that Mn³⁺ is kinetically trapped in tetrahedral sites and in a fully oxidized structure, consistent with the reduction of coordination number observed in EXAFS. Although in a reduced state, computation shows that Mn³⁺ states are stabilized relative to those of oxygen and that the highest occupied molecular orbital (HOMO) is thus dominated by oxygen states. Furthermore, the Mn³⁺(T_d) induces local strain on the oxide sublattice as observed in Raman spectra and results in a reduced gap between the HOMO and the lowest unoccupied molecular orbital (LUMO). As a result, the confluence of a reduced HOMO–LUMO gap and oxygen-based HOMO results in the facilitation of OER on the application of anodic potentials to the δ-MnO₂ polymorph incorporating Mn³⁺ ions.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Next Generation of Materials by Design: Incorporating Metastability (CNGMD); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

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

Grant/Contract Number:: AC36-08GO28308; AC02-76SF00515; 1541959; AC02-05CH11231

OSTI ID:: 1438083

Alternate ID(s):: OSTI ID: 1458415; OSTI ID: 1485097

Journal Information:: Proceedings of the National Academy of Sciences of the United States of America, Vol. 115, Issue 23; ISSN 0027-8424

Publisher:: National Academy of Sciences, Washington, DC (United States)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 178 works

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Synergistic Control of Structural Disorder and Surface Bonding Nature to Optimize the Functionality of Manganese Oxide as an Electrocatalyst and a Cathode for Li–O ₂ Batteries Jin, Xiaoyan; Park, Mihui; Shin, Seung‐Jae Small, Vol. 16, Issue 12 https://doi.org/10.1002/smll.201903265	journal	March 2020
Nickel‐Doping Effect on Mn ₃ O ₄ Nanoparticles for Electrochemical Water Oxidation under Neutral Condition Hong, Jung Sug; Seo, Hongmin; Lee, Yoon Ho Small Methods, Vol. 4, Issue 3 https://doi.org/10.1002/smtd.201900733	journal	January 2020
Manganese( ii ) phosphate nanosheet assembly with native out-of-plane Mn centres for electrocatalytic water oxidation Liu, Hongfei; Gao, Xueqing; Yao, Xiaolong Chemical Science, Vol. 10, Issue 1 https://doi.org/10.1039/c8sc03764g	journal	January 2019
A comparative study of metal (Ni, Co, or Mn)-borate catalysts and their photodeposition on rGO/ZnO nanoarrays for photoelectrochemical water splitting Zhang, Huayang; Tian, Wenjie; Li, Yunguo Journal of Materials Chemistry A, Vol. 6, Issue 47 https://doi.org/10.1039/c8ta06921b	journal	January 2018
Tunable nano-interfaces between MnO _x and layered double hydroxides boost oxygen evolving electrocatalysis Xue, Yudong; Fishman, Zachary S.; Röhr, Jason A. Journal of Materials Chemistry A, Vol. 6, Issue 44 https://doi.org/10.1039/c8ta07508e	journal	January 2018
“Switching on” iron in clay minerals Ilgen, A. G.; Kukkadapu, R. K.; Leung, K. Environmental Science: Nano, Vol. 6, Issue 6 https://doi.org/10.1039/c9en00228f	journal	January 2019
Origin of the heat-induced improvement of catalytic activity and stability of MnO _x electrocatalysts for water oxidation Abrashev, Miroslav V.; Chernev, Petko; Kubella, Paul Journal of Materials Chemistry A, Vol. 7, Issue 28 https://doi.org/10.1039/c9ta05108b	journal	January 2019
Thermally driven phase transition of manganese oxide on carbon cloth for enhancing the performance of flexible all-solid-state zinc–air batteries Chen, Song; Shu, Xinxin; Wang, Huaisheng Journal of Materials Chemistry A, Vol. 7, Issue 34 https://doi.org/10.1039/c9ta05719f	journal	January 2019
Albumin-stabilized manganese-based nanocomposites with sensitive tumor microenvironment responsivity and their application for efficient SiRNA delivery in brain tumors Xu, Kai; Zhao, Zhenghuan; Zhang, Junfeng Journal of Materials Chemistry B, Vol. 8, Issue 7 https://doi.org/10.1039/c9tb02341k	journal	January 2020
Metal-Organic Frameworks-Based Electrocatalysis: Insight and Future Perspectives Li, Xinlin; Maindan, Karan; Deria, Pravas Comments on Inorganic Chemistry, Vol. 38, Issue 5 https://doi.org/10.1080/02603594.2018.1545225	journal	September 2018
Electrochemical Analysis for Enhancing Interface Layer of Spinel LiNi0.5Mn1.5O4 Using p-Toluenesulfonyl Isocyanate as Electrolyte Additive Xiao, Zhe; Wang, Renheng; Li, Yan Frontiers in Chemistry, Vol. 7 https://doi.org/10.3389/fchem.2019.00591	journal	August 2019
Unpaired 3d Electrons on Atomically Dispersed Cobalt Centres in Coordination Polymers Regulate both Oxygen Reduction Reaction (ORR) Activity and Selectivity for Use in Zinc–Air Batteries Lian, Yuebin; Yang, Wenjuan; Zhang, Chufeng Angewandte Chemie International Edition, Vol. 59, Issue 1 https://doi.org/10.1002/anie.201910879	journal	November 2019
Non-equilibrium crystallization pathways of manganese oxides in aqueous solution Sun, Wenhao; Kitchaev, Daniil A.; Kramer, Denis Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-08494-6	journal	February 2019
A multi-technique approach for studying Na triclinic and hexagonal birnessites Boumaiza, Hella; Renard, Aurélien; Rakotomalala Robinson, Mbolantenaina Journal of Solid State Chemistry, Vol. 272 https://doi.org/10.1016/j.jssc.2019.02.017	journal	April 2019
Manganese( ii ) phosphate nanosheet assembly with native out-of-plane Mn centres for electrocatalytic water oxidation Liu, Hongfei; Gao, Xueqing; Yao, Xiaolong Chemical Science, Vol. 10, Issue 1 https://doi.org/10.1039/c8sc03764g	journal	January 2019

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