Sustainable H2O2 production via solution plasma catalysis

• 成果类型: Article
• 署名作者: Liang, Shuang; Wu, Qi; Wang, Changhua; Wang, Rui; Li, Dashuai; Xing, Yanmei; Jin, Dexin; Ma, He; Liu, Yichun; Zhang, Peng; Zhang, Xintong
• 署名单位: Northeast Normal University - China; Dalhousie University
• 刊物名称: PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
• ISSN/ISSBN: 0027-15132
• DOI: 10.1073/pnas.2410504121
• 发表日期: 2024-08-20
• 关键词: electrochemical synthesis; hydrogen-peroxide; singlet oxygen; water; degradation; surface; phenol

摘要

Clean production of hydrogen peroxide (H2O2) with water, oxygen, and renewable energy is considered an important green synthesis route, offering a valuable substitute for the traditional anthraquinone method. Currently, renewable energy-driven production of H2O2 mostly relies on soluble additives, such as electrolytes and sacrificial agents, inevitably compromising the purity and sustainability of H2O2. Herein, we develop a solution plasma catalysis technique that eliminates the need for soluble additives, enabling eco- friendly production of concentrated H2O2 directly from water and O2. Screening over 40 catalysts demonstrates the superior catalytic performance of carbon nitride interacting with discharge plasma in water. High- throughput density functional theory calculations for 68 models, along with machine learning using 29 descriptors, identify cyano carbon nitride (CCN) as the most efficient catalyst. Solution plasma catalysis with the CCN achieves concentrated H2O2 of 20 mmol L-1, two orders of magnitude higher than photocatalysis by the same catalyst. Plasma diagnostics, isotope labeling, and COMSOL simulations collectively validate that the interplay of solution plasma and the CCN accounts for the significantly increased production of singlet oxygen and H2O2 thereafter. Our findings offer an efficient and sustainable pathway for H2O2 production, promising wide- ranging applications across the chemical industry, public health, and environmental remediation.