文献类型：期刊文献

英文题名：Electrocatalytic Production of H2O2 by Selective Oxygen Reduction Using Earth-Abundant Cobalt Pyrite (CoS2)

作者：Sheng, Hongyuan[1];Hermes, Eric D.[1];Yang, Xiaohua[1,2];Ying, Diwen[1,3];Janes, Aurora N.[1];Li, Wenjie[1];Schmidt, J. R.[1];Jin, Song[1]

机构：[1]Univ Wisconsin, Dept Chem, 1101 Univ Ave, Madison, WI 53706 USA;[2]East China Univ Sci & Technol, Sch Mat Sci & Engn, Minist Educ, Key Lab Ultrafine Mat, 130 Meilong Rd, Shanghai 200237, Peoples R China;[3]Shanghai Jiao Tong Univ, Sch Environm Sci & Engn, 800 Dongchuan Rd, Shanghai 200240, Peoples R China

年份：2019

卷号：9

期号：9

起止页码：8433

外文期刊名：ACS CATALYSIS

收录：;EI(收录号：20193607402829);WOS:【SCI-EXPANDED(收录号:WOS:000485090400081)】；

基金：This research was partially supported by the National Science Foundation (NSF) Grant DMR-1508558 (H.S., W.L., and S.J.) for the material synthesis, by University of Wisconsin-Madison and King Abdullah University of Science and Technology (KAUST) OSR-2017-CRG6-3453.02 (H.S., W.L., and S.J.) for the electrochemical characterization, and CHE-1362136 (E.D.H, A.N.J., and J.R.S.) for the theoretical calculation. X.Y. and D.Y. thank the China Scholarship Council (CSC) and the National Natural Science Foundation of China (NSFC) Grant 51608319 for support. The authors gratefully acknowledge use of facilities and instrumentation supported by NSF through the University of Wisconsin Materials Research Science and Engineering Center (DMR-1720415).

语种：英文

外文关键词：selective electrocatalysis; oxygen reduction; hydrogen peroxide; earth-abundant; pyrite

摘要：Decentralized on-site production of hydrogen peroxide (H2O2) relies on efficient, robust, and inexpensive electrocatalysts for the selective two-electron (2e(-)) oxygen reduction reaction (ORR). Here, we combine computations and experiments to demonstrate that cobalt pyrite (CoS2), an earth-abundant transition-metal compound, is both active and selective toward 2e(-) ORR in the acidic solution. CoS2 nanomaterials drop-casted on the rotating ring-disk electrode (RRDE) showed selective and efficient H2O2 formation in 0.05 M H2SO4 at high catalyst loadings, with their operational stability evaluated by structural and surface analyses. CoS2 nanowires directly grown on the high-surface-area carbon fiber paper electrode boosted the overall performance of bulk ORR electrolysis and the H2O2 product was chemically quantified to yield a similar to 70% H2O2 selectivity at 0.5 V vs reversible hydrogen electrode (RHE), in good agreement with the RRDE results. Computations suggested the modest binding of OOH* adsorbate on the single Co site of CoS2 and the kinetically disfavored O-O bond scission due to the lack of active site ensembles in the crystal structure, consistent with the experimentally observed activity and selectivity. CoS2 also catalyzes 2e(-) ORR with less activity and selectivity in the noncorrosive neutral solution. This work opens up the exploration of diverse earth-abundant transition-metal compounds in search of highly active and selective electrocatalysts for efficient H2O2 production.