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CHEMICAL ENGINEERING JOURNAL · 2025 · IF 13.2

Boosting molecular oxygen activation through synergistic interaction of boron-doped biochar and ascorbic acid: Key role of BC2O and BC3

Qingyang Dai,Kecheng Zhu,Yongliang Xu,Yixuan Liu,Yuanren Jiang,Chenghe Yan,Chi Zhang,Hanzhong Jia

Ambiguous interpretations regarding the underlying mechanism of molecular oxygen (O 2 ) activation by the carbonaceous material/reductant system, especially in terms of the catalytic active site, have impeded the optimization and broader application of the system in environmental remediation. Here, we thoroughly investigated the role of boron-doped biochar (BBC) active sites in O 2 activation and optimized the ascorbic acid (AA) dosing strategy to improve the hydroxyl radical (•OH) production rate and pollutant removal. The introduction of boron facilitated O 2 activation through the successive one-electron transfer to generate •OH that predominantly occurred and accumulated on BBC surface, where •OH yield was nearly 5-fold and 9-fold higher than that in N-doped biochar/AA and zero-valence iron (ZVI) system, respectively. This results in better degradation performance of BBC/AA system for organic pollutants absorbed on the BBC surface and robust resistance to commonly occurring water anions and negatively charged organic matter. Moreover, the stepwise addition of low-concentration AA (0.5 mM) promoted the BPA removal (over 90 %) by maximizing the effective availability of AA and •OH. Characterization, galvanic oxidation process, and theory calculation results revealed that BC 2 O acted as the primary electron-accepting group to receive the electrons from AA, while BC 3 acted as both an electron-donating group and an O 2 adsorption site on BBC, which together facilitated O 2 activation and •OH production on the BBC surface. These findings provide a comprehensive understanding of O 2 activation within the BBC/AA system, highlighting its potential as a sustainable and effective approach for advanced environmental remediation applications.

研究领域: 环境科学 · 材料科学
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2022 · IF 24.319

Reveals that electron transfer regime mediated by electron shuttle rather than adjacent transfer in B-doped 3D porous carbon framework: Exploration of interactions and identification of the main active site

Meng-Zhu Qin,Yanyan Bian,Huai-Yuan Niu,Wen-Xin Fu,Xue-Gang Zhang,Qi-Yao Hu,Duan Guo,Cheng-Gang Niu,Lei Zhang

The determination of non-radical pathways and identification of the main active site in the persulfate (PS) activation by B-doped carbonaceous materials are still controversial. Therefore, sodium citrate was selected as the carbon source and self-template for synthesizing a B-doped carbonaceous materials to activate peroxydisulfate (PDS) in this work. Multiple characterizations and experiments revealed that the electron transfer regime was responsible for the activation of PDS. On the one hand, the metastable surface complexes were generated due to the adsorption of PDS onto the catalyst surface via inner-sphere interaction. On the other hand, the interaction between BPA and the catalyst was verified as charge-assisted hydrogen bonding. In addition, BC 3 was identified as the main active site. Based on the detailed and in-depth exploration of the electron transfer regime during the PDS activation of B-doped carbonaceous materials, this work further elucidated interactions, and the vital role of BC 3 in PDS activation.

CAS / MDL: 98-00-0
研究领域: 材料科学 · 环境化学 · 催化
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