Journal
CHEMCATCHEM
Volume 11, Issue 24, Pages 6051-6060Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cctc.201901224
Keywords
dual doping; iron nitride; interface engineering; d-band center; overall water splitting
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Funding
- Natural Science Foundation of China [21875292, 21706295, 21773315]
- Fundamental Research Funds for the Central Universities [17lgjc36]
- Natural Science Foundation of Guangdong Province [2017A030313055]
- Guangdong Provincial Key Platform and Major Scientific Research Projects for Colleges and Universities [2015KCXTD029]
- Science and Technology Plan Project of Guangzhou, China [201804020025]
- Science Starting Foundation of Hunan University [531118010182]
- China Postdoctoral Science Foundation [2018M640847, 2019T120764]
- Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program
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Interfacial engineering and electronic modulation are some of the main components for enhancing the catalytic activity of electrocatalysts towards achieving efficient water splitting. Iron nitrides exhibit mediocre oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) due to their unsuitable d-band energy level. In this work, we strongly boost the HER and OER catalytic performance of Fe2N for the first time by doping Co and Al, which could not only induce the formation of Fe2N/Fe3N hybrid interface but also tune the d-band center position. The CoAl-Fe2N/Fe3N nanoparticles display HER and OER overpotential of 145 and 307 mV at 10 mA/cm(2). XPS and DFT calculations confirm that tailoring the d-band center position and interfacial engineering facilitates strong electronic interactions between Fe2N and Fe3N, synergistically optimize the electronic structure, which enriches H and H2O adsorption energy and oxygen-containing intermediates. An alkaline electrolyzer based on CoAl-Fe2N/Fe3N requires an overall potential of 1.67 V at 10 mA/cm(2), demonstrating the use of iron nitrides as a bifunctional electrocatalyst for water splitting activity.
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