期刊
ACS CATALYSIS
卷 11, 期 2, 页码 509-516出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.0c04102
关键词
ammonia electrosynthesis; local modulation; single-atom catalyst; Mn sites; ambient condition; N-2 reduction reaction
资金
- National Key R&D Program of China [2017YFA0700104]
- National Natural Science Foundation of China [22075211, 21601136, 51971157, 51761165012]
- Tianjin Science Fund for Distinguished Young Scholars [19JCJQJC61800]
- Science and Technology Development Fund of Tianjin Education Commission for Higher Education [2018KJ126]
- DOE Office of Science [DE-SC0012704]
The study focuses on optimizing the local structures of single-atomic active sites for the N-2 reduction reaction through controlling Mn-O bonding conditions. By constructing single Mn-O3N1 sites anchored on porous carbon, an enhanced NH3 yield rate was achieved, attributed to unique geometry and electronic structures that facilitate N-2 molecule adsorption and activation.
Rationally tuning the local structures of single-atomtc active sites for the electrocatalytic N-2 reduction reaction (NRR) remains an urgent but worthwhile research topic. Herein, we accomplish the local modulation of single-atomic Mn sites and construct single Mn-O3N1 sites anchored on porous carbon Mn-O3N1/PC) by delicately controlling the Mn-O bonding conditions. The constructed structures are confirmed via the combination of atomic-scale imaging, Raman spectroscopy, synchrotron radiation-based soft and hard X-ray absorption spectroscopies, and X-ray photoelectron spectroscopy. The Mn-O3N1/PC catalyst yields an NH3 yield rate of 66.41 mu g h(-1) mg(cat)(-1) (corresponding to 1.56 mg h(-1) mg(cat)(-1)) at -0.35 V versus reversible hydrogen electrode, which is about four times that on the control Mn-N-4/PC catalyst. The enhanced NRR performance is ascribed to its unique geometry and electronic structures, which not only facilitate the adsorption and activation of the N-2 molecule but also lower the free energy change of the potential-determining step.
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