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Biochar aerogel decorated with thiophene S manipulated 5-membered rings boosts nitrogen fixation
Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2022-04-20 , DOI: 10.1016/j.apcatb.2022.121425
Xiaokang Chen, Lijie Zhang, Wenjia Xu, Xin Ding, Shuai Chen, Xilin She, Xiangxin Guo, Chung-Li Dong, Yucheng Huang, Lixue Zhang, Shaohua Shen, Dongjiang Yang

Algae contains most of the marine biogenic S, and is the main producer of dimethylsulfide, of which oxidation products contribute ~ 40% acidity of the acid rain. The biogenic S of red algae mainly exists in carrageenan molecules. In this work, 89% of C and 96% of biogenic S in carrageenan was synchronically fixed into biochar to form thiophene S decorated biochar aerogel (SCA), efficiently preventing the loss of C and S elements. More importantly, the presence of thiophene S structure in SCA can “push” electrons into the antibonding orbitals of N2, and simultaneously “pull” the lone-pair electrons from N2, thus endowing the SCA super activity for nitrogen reduction reaction. Experimentally, its NH3 yield rate reaches high as 36.69 μg h−1 mg−1cat, surpassing most metal-free electrocatalysts. Theoretical calculations demonstrate that the thiophene S can promote the absorption and activation of N2, and efficiently lower the energy barrier of N2 protonation.



中文翻译:

用噻吩 S 操纵的 5 元环装饰的生物炭气凝胶可促进固氮

藻类含有大部分海洋生物源硫,是二甲基硫醚的主要生产者,其中氧化产物贡献了约 40% 的酸雨酸度。红藻的生物源性S主要存在于卡拉胶分子中。在这项工作中,卡拉胶中 89% 的 C 和 96% 的生物源 S 同步固定在生物炭中,形成噻吩 S 修饰的生物炭气凝胶 (SCA),有效防止了 C 和 S 元素的损失。更重要的是,SCA中噻吩S结构的存在可以将电子“推”入N 2 的反键轨道同时从N 2中“拉”出孤对电子,从而赋予了SCA对氮还原反应的超强活性。经实验,其NH 3产率高达36.69 μg h -1mg -1 cat,超过大多数无金属电催化剂。理论计算表明,噻吩S可以促进N 2 的吸收和活化有效降低N 2质子化的能垒。

更新日期:2022-04-20
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