Co-catalysis of metal sulfides accelerating Fe2+/Fe3+ cycling for the removal of tetracycline in heterogeneous electro-Fenton using an novel rolled NPC/CB cathodes

Co-catalysis of metal sulfides accelerating Fe2+/Fe3+ cycling for the removal of tetracycline in heterogeneous electro-Fenton using an novel rolled NPC/CB cathodes
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DOI:
10.1016/j.seppur.2021.119200
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发表时间:
2021-07-01
影响因子:
8.6
通讯作者:
Ma, Hongrui
Ma, Hongrui
中科院分区:
工程技术1区
文献类型:
--
作者:
FangkeYu;Wang, Shuai;Ma, Hongrui

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以聚四氟乙烯(PTFE)为粘结剂,采用掺氮多孔炭(NPC)和炭黑(CB)制备了一种新型的滚压式碳质气体扩散阴极,通过优化,在近中性pH条件下,H2 O2的产率可达7.27 mg h(-1)cm(-2)。将NPC/CB阴极进一步应用于合成黄铁矿(FeS 2)为催化剂、金属硫化物(MoS 2、WS 2)为助催化剂的非均相电芬顿(EF)实验中,四环素(50 mg L-1)的去除率可达100%,对应物的总有机碳(TOC)去除率可达81.3%。由于FeS 2在H2 O2的存在下产生H+和Fe 2+,为EF提供了合适的pH值和催化离子。同时,金属硫化物通过暴露催化剂表面的可还原金属活性中心,加速了Fe 3+向Fe 2+的转化,从而大大提高了H2 O2的分解效率和污染物的降解效率,同时也改善了FeS 2在非均相EF中Fe 2+浸出少的缺点。对该系统的进一步测试表明,它具有处理制革废水的潜力。为促进异构EF系统的改进和实际应用的发展提供了一种有效可行的方案。
This work utilizes nitrogen-doped porous carbon (NPC) and carbon black (CB) to fabricate a novel rolled carbonaceous gas-diffusion cathode by polytetrafluoroethylene (PTFE) as adhesive, which greatly improves the production of H2O2 to 7.27 mg h(-1) cm(-2) by optimization in near neutral pH condition. Further application of NPC/CB cathode in heterogeneous electro-Fenton (EF) experiments with synthetic pyrite (FeS2) as catalyst, metal sulfides (MoS2, WS2) as co-catalysts, the removal efficiency of the tetracycline (50 mg L-1) could reach 100% and the total organic carbon (TOC) removal efficiency of counterpart could reach 81.3%, respectively. Because of the FeS2 produces H+ and Fe2+ in the presence of H2O2, which provides pH value and catalytic ion that suitable for EF. Meanwhile, the metal sulfides can accelerate the conversion of Fe3+ to Fe2+ by exposing reducible metal active sites on the surface of the catalysts, thus drastically increased the efficiency of H2O2 decomposition and pollutant degradation, also optimized the disadvantage of little Fe2+ leaching from FeS2 in heterogeneous EF. Further tests of this system indicated its potential for the treatment of tannery effluents. It provided an effective and feasible scheme for promoting the improvement of the heterogeneous EF system and the development of practical application.