Song Ge, Wu Huizhong, Wang Xuechun, Li Shuaishuai, Liang Ruiheng, Zhou Minghua
Key Laboratory of Pollution Process and Environmental Criteria, Ministry of Education, College of Environmental Science and Engineering, Nankai University, Tianjin 300350, China; Tianjin Key Laboratory of Environmental Technology for Complex Trans-Media Pollution, College of Environmental Science and Engineering, Nankai University, Tianjin 300350, China; Tianjin Advanced Water Treatment Technology International Joint Research Center, College of Environmental Science and Engineering, Nankai University, Tianjin 300350, China.
Key Laboratory of Pollution Process and Environmental Criteria, Ministry of Education, College of Environmental Science and Engineering, Nankai University, Tianjin 300350, China; Tianjin Key Laboratory of Environmental Technology for Complex Trans-Media Pollution, College of Environmental Science and Engineering, Nankai University, Tianjin 300350, China; Tianjin Advanced Water Treatment Technology International Joint Research Center, College of Environmental Science and Engineering, Nankai University, Tianjin 300350, China.
J Hazard Mater. 2024 Aug 5;474:134750. doi: 10.1016/j.jhazmat.2024.134750. Epub 2024 May 28.
Electrocatalytic dechlorination by atomic hydrogen (H*) is efficient, but limited by the low efficiency of H* production. Herein, a phosphorus-doped cobalt nitrogen carbon catalyst (Co-NP/C) was prepared, which had high catalytic activity in a wide pH range (3-11). The turnover frequency of Co-NP/C (3.54 min) was 1.21-59000 times superior to that of current Pd-based and non-noble metal catalysts (0.00006-2.92 min). Co-NP/C significantly enhanced H* generation, which was 1.52, 2.44, and 3.77 times stronger than that of Co-N/C, NP/C, and N/C, respectively, since the introduction of phosphorus was found enhanced the electron density of cobalt and regulated the electron transfer. Co-NP/C showed outstanding catalytic performance after ten cycles and could achieve nearly complete chloramphenicol removal. This regulation method was verified to be effective for other non-noble metal (Fe, Mn, Cu, Ni) phosphorus doped catalysts, proposing a general class for efficient electrochemical dechlorination, which would be of great significance for the elimination of chlorinated organic pollutants.
原子氢（H*）介导的电催化脱氯效率很高，但受限于H生成效率较低。在此，制备了一种磷掺杂的钴氮碳催化剂（Co-NP/C），其在较宽的pH范围（3-11）内具有高催化活性。Co-NP/C的周转频率（3.54 min⁻¹）比目前的钯基和非贵金属催化剂（0.00006-2.92 min⁻¹）高1.21-59000倍。Co-NP/C显著增强了H的生成，分别比Co-N/C、NP/C和N/C强1.52、2.44和3.77倍，因为发现引入磷提高了钴的电子密度并调节了电子转移。Co-NP/C在十个循环后表现出出色的催化性能，并且可以实现氯霉素的近乎完全去除。这种调控方法被证明对其他非贵金属（Fe、Mn、Cu、Ni）磷掺杂催化剂有效，提出了一类高效电化学脱氯的通用方法，这对于消除氯代有机污染物具有重要意义。
