Regulating the electronic structure by P-doping cobalt-based catalyst for atomic hydrogen mediated electrocatalytic dechlorination

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-1) was 1.21-59000 times superior to that of current Pd-based and non-noble metal catalysts (0.00006-2.92 min-1). 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. 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). Co-NP/C significantly enhanced H* generation. The turnover frequency of Co-NP/C was 1.21-59000 times superior to that of current Pd-based and non-noble metal catalysts. This regulation method was verified to be effective for other non-noble metal (Fe, Mn, Cu, Ni) phosphorus doped catalysts, which would be of great significance for the elimination of chlorinated organic pollutants.