Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2023-06-17 , DOI: 10.1016/j.apcatb.2023.123018
Qiang Yang , Longgang Chu , Tongliang Wu , Yiyi Zhou , Cun Liu , Long Cang , Guodong Fang , Peixin Cui , Yujun Wang
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In heterogeneous electro-Fenton process, the design of electrocatalysts for in-situ generation of H2O2 and efficient conversion to •OH remains a challenge. Herein, a simple one-step pyrolysis strategy has been developed to synthesize green and stable dual-functional electro-catalysts from agricultural wastes. The biochar of soybean roots (RSBC) with ample -COOH and C-O-C functional groups exhibited considerable capacity for H2O2 production (21.6 mM at −0.4 V vs RHE), and the dual-functional electron-catalyst exhibits an excellent catalytic reaction for antibiotics removal (100 % cloroquine phosphate with kobs=0.035 min−1). The ultra-small MnO nanoclusters (<2 nm) in the biochar of Phytolacca americana leaves (LPBC) were the active center via the transfer of electrons between adsorbed H2O2 and Mn atoms to produce reactive •OH, as identified by operando X-ray absorption fine structure (XAFS) spectroscopy and density functional theory calculations. This work provides a new direction in the design of dual-functional carbon cathode catalysts for environmental remediation.
中文翻译:

非均相电芬顿过程中农业废弃物双功能碳阴极催化剂的研究
在非均相电芬顿过程中,原位产生H 2 O 2并有效转化为•OH的电催化剂设计仍然是一个挑战。在此,开发了一种简单的一步热解策略,从农业废物中合成绿色且稳定的双功能电催化剂。具有丰富的-COOH和COC官能团的大豆根生物炭(RSBC)表现出相当大的H 2 O 2生产能力(-0.4 V vs RHE时为21.6 mM),并且双功能电子催化剂表现出优异的催化反应抗生素去除(100% 磷酸氯喹,k obs =0.035 min −1)。美洲商陆叶 (LPBC)生物炭中的超小 MnO 纳米团簇 (<2 nm)是活性中心,通过吸附的 H 2 O 2和 Mn 原子之间的电子转移产生反应性·OH,如操作X所示-射线吸收精细结构(XAFS)光谱和密度泛函理论计算。这项工作为环境修复双功能碳阴极催化剂的设计提供了新的方向。