PMID- 31393100 OWN - NLM STAT- PubMed-not-MEDLINE LR - 20190906 IS - 1944-8252 (Electronic) IS - 1944-8244 (Linking) VI - 11 IP - 35 DP - 2019 Sep 4 TI - Facile Preparation of Carbon Shells-Coated O-Doped Molybdenum Carbide Nanoparticles as High Selective Electrocatalysts for Nitrogen Reduction Reaction under Ambient Conditions. PG - 31869-31877 LID - 10.1021/acsami.9b09007 [doi] AB - Electrochemical nitrogen reduction reaction (NRR) has been considered as a promising alternative to the traditional Haber-Bosch process for the preparation of ammonia (NH(3)) under ambient conditions. The development of cost-effective electrocatalysts with suppressive activity for hydrogen evolution reaction is critical for improving the efficiency of NRR. Herein, oxygen-containing molybdenum carbides (O-MoC) embedded in nitrogen-doped carbon layers (N-doped carbon) can be easily fabricated by pyrolyzing the chelate of dopamine and molybdate. A rate of NH(3) formation of 22.5 mug.h(-1).mg(cat)(-1) is obtained at -0.35 V versus reversible hydrogen electrode with a high faradaic efficiency of 25.1% in 0.1 mM HCl + 0.5 M Li(2)SO(4). Notably, the synthesized O-MoC@NC-800 also exhibits high selectivity (no formation of hydrazine) and electrochemical stability. The moderate electron structure induced by the interaction between O-MoC and N-doped carbon shells can effectively weaken the activity of hydrogen evolution reaction and increase the faradaic efficiency of NRR. Additionally, by applying the in situ Fourier transform infrared spectroscopy, an associative reaction pathway is proposed on O-MoC@NC-800. This work provides new insights into the rational design of carbon-encapsulated metal nanoparticles as efficient catalysts for NRR at ambient conditions. FAU - Qu, Ximing AU - Qu X AD - State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering , Xiamen University , Xiamen 361005 , People's Republic of China. FAU - Shen, Linfan AU - Shen L AD - State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering , Xiamen University , Xiamen 361005 , People's Republic of China. FAU - Mao, Yujie AU - Mao Y AD - State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering , Xiamen University , Xiamen 361005 , People's Republic of China. FAU - Lin, Jinxia AU - Lin J AD - State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering , Xiamen University , Xiamen 361005 , People's Republic of China. FAU - Li, Yuyang AU - Li Y AD - State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering , Xiamen University , Xiamen 361005 , People's Republic of China. FAU - Li, Guang AU - Li G AD - State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering , Xiamen University , Xiamen 361005 , People's Republic of China. FAU - Zhang, Yuyang AU - Zhang Y AD - State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering , Xiamen University , Xiamen 361005 , People's Republic of China. FAU - Jiang, Yanxia AU - Jiang Y AUID- ORCID: 0000-0002-8633-4460 AD - State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering , Xiamen University , Xiamen 361005 , People's Republic of China. FAU - Sun, Shigang AU - Sun S AUID- ORCID: 0000-0003-2327-4090 AD - State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering , Xiamen University , Xiamen 361005 , People's Republic of China. LA - eng PT - Journal Article DEP - 20190820 PL - United States TA - ACS Appl Mater Interfaces JT - ACS applied materials & interfaces JID - 101504991 SB - IM OTO - NOTNLM OT - N-doped carbon shells OT - electrocatalysis OT - molybdenum carbides OT - nitrogen reduction reaction OT - selectivity EDAT- 2019/08/09 06:00 MHDA- 2019/08/09 06:01 CRDT- 2019/08/09 06:00 PHST- 2019/08/09 06:00 [pubmed] PHST- 2019/08/09 06:01 [medline] PHST- 2019/08/09 06:00 [entrez] AID - 10.1021/acsami.9b09007 [doi] PST - ppublish SO - ACS Appl Mater Interfaces. 2019 Sep 4;11(35):31869-31877. doi: 10.1021/acsami.9b09007. Epub 2019 Aug 20.