Wang Xinyu, Shen Wangqiang, Zhang Chang, Huang Yuzhong, Zhang Jian, Lv Jun, Lu Xing
School of Materials Science and Engineering, Hefei University of Technology, Hefei, Anhui, 230009, China.
School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan, Hubei, 430074, China.
Angew Chem Int Ed Engl. 2025 Feb 10;64(7):e202419049. doi: 10.1002/anie.202419049. Epub 2024 Dec 2.
Developing seawater-compatible hydrogen peroxide (HO) electroproduction technologies is crucial for advancing marine resource utilization in coastal regions. However, designing efficient and highly stable non-noble metal catalysts for two-electron oxygen reduction reaction (2e ORR) in seawater environment remains a challenging task due to the corrosive and toxic nature of chloride ions (Cl). Herein, we present, for the first time, a novel nitrogen and oxygen self-doped defect-rich nanocarbon (NO-DC) catalyst, derived from silk fiber, which addresses these challenges with low toxicity, cost-effectiveness, and high adaptability. The obtained NO-DC catalyst demonstrates an impressive HO production rate of up to 4997 mg L h, a high Faradaic efficiency of 96.5 %, and produces 4.3 wt % HO after 20 hours of stable operation, placing it among the highest-performing catalysts reported in neutral electrolytes. Theoretical calculations reveal that NO-DC's superior 2e ORR performance is due to the synergistic effect of graphitic nitrogen and C-OH, which inhibits Cl adsorption and promotes *OOH adsorption. Additionally, integrating 2e ORR with Fenton-like technology enables rapid degradation of organic pollutants and effective inactivation of seawater algae, offering significant potential for mitigating coastal eutrophication and red tide pollution. This work provides valuable insights into HO electrosynthesis in seawater solution and promises advancements in ocean-energy applications.
开发与海水兼容的过氧化氢(HO)电生产技术对于推进沿海地区的海洋资源利用至关重要。然而,由于氯离子(Cl)具有腐蚀性和毒性,设计用于海水中双电子氧还原反应(2e ORR)的高效且高度稳定的非贵金属催化剂仍然是一项具有挑战性的任务。在此,我们首次展示了一种源自丝纤维的新型氮氧自掺杂富含缺陷的纳米碳(NO-DC)催化剂,它以低毒性、成本效益高和适应性强应对了这些挑战。所获得的NO-DC催化剂表现出高达4997 mg L h的过氧化氢产率、96.5 %的高法拉第效率,并且在稳定运行20小时后产生4.3 wt %的过氧化氢,使其跻身中性电解质中报道的性能最佳的催化剂之列。理论计算表明,NO-DC优异的2e ORR性能归因于石墨氮和C-OH的协同效应,该效应抑制了Cl的吸附并促进了*OOH的吸附。此外,将2e ORR与类芬顿技术相结合能够快速降解有机污染物并有效灭活海水藻类,为缓解沿海富营养化和赤潮污染提供了巨大潜力。这项工作为海水中过氧化氢的电合成提供了有价值的见解,并有望推动海洋能源应用的发展。