期刊
CARBON ENERGY
卷 4, 期 2, 页码 237-245出版社
WILEY
DOI: 10.1002/cey2.160
关键词
biosynthesis; carbon-based materials; chromium phosphide; leachate treatment; nitrogen reduction reaction; resource recovery
类别
资金
- Taishan Scholars Project Special Funds [tsqn201812083]
- Natural Science Foundation of Shandong Province [ZR2019YQ20, 2019JMRH0410]
- National Natural Science Foundation of China [51972147, 52022037, 52002145]
The synthesis of CrP/NPC nanoparticles through consecutive leachate treatment and resource recovery process shows excellent nitrogen reduction reaction performance and catalytic stability. Experimental results confirm the efficient production of NH3 from the NRR process using CrP/NPC. DFT calculations reveal the crucial role of the electron deficiency environment of the Cr site in promoting the NRR process.
The resource recovery of heavy metals from effluent has significant environmental implications and potential commercial value. Chromium phosphide nanoparticles embedded in a nitrogen-/phosphorus-doped porous carbon matrix (CrP/NPC) are synthesized via a consecutive Cr6+ leachate treatment and resource recovery process. Electrochemical testing shows that CrP/NPC shows excellent nitrogen reduction reaction (NRR) performance, which yields the highest NH3 production rate of 22.56 mu g h(-1) mg(cat.)(-1) and Faradaic efficiency (16.37%) at -0.5 V versus the reversible hydrogen electrode in a 0.05 M Na2SO4 aqueous solution, as well as robust catalytic stability. The isotopic experiments using N-15(2) as a nitrogen source confirm that the detected NH3 is derived from the NRR process. Finally, density functional theory (DFT) calculations show that the electron deficiency environment of the Cr site can significantly reduce the barrier of the NRR process and promote the formation of intermediate species.
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