| 학회 |
한국재료학회 |
| 학술대회 |
2021년 봄 (05/12 ~ 05/14, 광주 김대중컨벤션센터) |
| 권호 |
27권 1호 |
| 발표분야 |
특별심포지엄 5. 에너지 변환소재 심포지엄-오거나이저: 심욱(전남대) |
| 제목 |
Selective electrochemical NO-to-NH2OH conversion catalyzed by isolated Fe catalyst |
| 초록 |
Electrocatalytic conversion of nitrogen oxides to value-added chemicals is a promising strategy for mitigating the human-caused unbalance of the global nitrogen-cycle, but controlling product selectivity remains a great challenge. Here we show iron-nitrogen-doped carbon as an efficient and durable electrocatalyst for selective nitric oxide reduction into hydroxylamine. Using in operando spectroscopic techniques, catalytic site is identified as isolated ferrous moieties, at which the rate for hydroxylamine production increases in a super-Nernstian way upon pH decrease. Computational multi-scale modeling attributes the origin of unconventional pH dependence to the redox active (non-innocent) property of NO. This makes the rate-limiting NO adsorbate state more sensitive to surface charge which varies with the pH-dependent overpotential. Guided by these fundamental insights, we achieve a Faradaic efficiency of 71% and an unprecedented production rate of 215 μmol cm−2 h−1 at a short-circuit mode in a flow-type fuel cell without significant catalytic deactivation over 50 h operation. |
| 저자 |
최창혁 |
| 소속 |
GIST |
| 키워드 |
Electrocatalysis; nitrogen cycle; single-atom metal catalyst; nitric oxide; hydroxylamine
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| E-Mail |
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