期刊
JOURNAL OF MATERIALS CHEMISTRY A
卷 7, 期 20, 页码 12627-12634出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c9ta02045d
关键词
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资金
- Chinese Academy of Sciences [YZ201627]
- National Natural Science Foundation of China (NSFC) [51801205, 11674321, 51571186, 11504375]
- China Postdoctoral Science Foundation [2018M632559]
- Chinese Academy of Sciences/State Administration of Foreign Experts Affairs (CAS/SAFEA) International Partnership Program for Creative Research Teams
Due to the strong absorbability and excellent activating ability of palladium (Pd) element for N-2, Pd-based materials have become one of the most promising catalysts for electrocatalytic N-2 reduction reaction (NRR) applications, which is a low-cost and ecofriendly way for ammonia synthesis under ambient conditions. However, the lack of active sites and poor stability are still the major issues that restrain their catalytic activity. To solve these problems, PdO/Pd heterojunctions supported on carbon nanotubes (PdO/Pd/CNTs) with a controllable mass ratio of Pd to PdO were fabricated using ultraviolet laser irradiated PdO/CNTs in distilled water. Compared with PdO/CNTs, PdO/Pd/CNTs, especially the ten minutes irradiated one, present an optimal mass ratio of Pd (18%) to PdO (82%) and abundant PdO-Pd interfaces which can act as active sites for N-2 dynamic activation and proton transitions, where the synergistic effect of Pd and PdO contributed to shorten the transmission route of protons and reduce the overpotential of the chemical reaction. Thus, the N-2 conversion efficiency of PdO/Pd/CNTs was obviously improved, their faradaic efficiency reached up to 11.5% and NH3 yield was 18.2 g mg(cat.)(-1) h(-1) at 0.1 V vs. RHE. Besides, this work will provide useful reference to design NRR catalysts with controllable surface states and defects by laser-assisted strategies.
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