A Cu and Fe dual-atom nanozyme mimicking cytochrome c oxidase to boost the oxygen reduction reaction. Issue 33 (11th August 2020)

• Record Type: Journal Article
• Authors: Du, Cheng; Gao, Yijing; Chen, Hengquan; Li, Ping; Zhu, Shuyun; Wang, Jianguo; He, Qinggang; Chen, Wei
• Is Part Of: Journal of materials chemistry. Volume 8:Issue 33(2020)
• Page Start: 16994
• Page End: 17001
• Publication Date: 2020-08-11
• Subjects: Materials -- Research -- Periodicals; Chemistry, Analytic -- Periodicals; Environmental sciences -- Research -- Periodicals; 543.0284
• DOI: 10.1039/d0ta06485h
• Languages: English
• ISSNs: 2050-7488

Abstract

Abstract : Through mimicking cytochrome c oxidase, the fabricated Cu and Fe dual-atom nanozyme exhibits enhanced catalytic performance for the oxygen reduction reaction. Abstract : The intrinsically sluggish kinetics of the oxygen reduction reaction (ORR) and overuse of expensive and unstable Pt-based catalysts have severely hampered the development of clean energy technologies. Herein, a type of non-noble metal nanozyme as an ORR electrocatalyst, with Fe–Cu dual atomic sites embedded in three-dimensional porous N-doped carbon (FeCu-DA/NC), is fabricated by mimicking both the constituents of active centers and enzymatic microenvironment of Cytochrome c oxidase (CcO). The atomically dispersed Fe–Cu single atom sites are clearly identified by direct aberration-corrected transmission electron microscopy imaging, systematic X-ray absorption fine structure (XAFS) analyses, and density functional theory (DFT) calculations. FeCu-DA/NC exhibits a superior ORR activity, with about 30 mV more positive half-wave potential ( E 1/2 ) than that of commercial Pt/C catalysts in a base, and moreover with only an E 1/2 gap of 20 mV to Pt/C in an acid. Importantly, FeCu-DA/NC displays an excellent durability under both acidic and basic conditions, which is much superior to that of Pt/C. DFT calculations further demonstrate that the enhanced performance can be attributed to the unique synergistic effect between Cu and Fe single atoms in which Cu–N4 serves as the electron donor to increase the electron density of the active centers of Fe–N4 and thus to facilitate O2 activation.