Unravelling the Functional Complexity of Oxygen-containing Groups on Carbon for the Reduction of NO with NH3
Unravelling the Functional Complexity of Oxygen-containing Groups on Carbon for the Reduction of NO with NH3
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揭示碳上含氧基团用于用 NH3 还原 NO 的功能复杂性
DOI：
10.1016/j.jtice.2022.104261
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发表时间：
2022-04
影响因子：
5.7
通讯作者：
Jian-guo Wang
中科院分区：
文献类型：
--
作者：
Yuran Li;Shijie Zhang;Xiujuan Sun;Chun Wang;Xiangyu Kong;Lili Zhang;Xing Zhong;Shangpeng Zhai;Zihao Yao;Jian-guo Wang
背景碳材料上的含氧基团在热催化和电催化反应中起着至关重要的作用。采用过氧化氢氧化法合成了一系列不同含氧基团的碳基催化剂，用于NH3选择性催化还原NO。方法采用氮气吸附-脱附和光谱表征方法对催化剂的织构性质和含氧基团类型进行了表征。反硝化实验结果表明，反硝化效率与含氧量相关。密度泛函理论(DFT)计算表明，含氧基团可以促进NO和NH3的化学吸附，从而获得较高的NO还原性能。有意义的发现碳材料上的羧基和苯酚基团有利于催化脱氮性能。此外，根据机理分析认为，CO(NH4)和C(NO)在表面氧化物上的形成是NH3还原NO的重要步骤。我们的发现为在相对较低的温度下设计和合成具有良好的含氧碳材料活性的SCR催化剂提供了新的策略。
BackgroundOxygen-containing groups on carbon materials play a crucial role in thermocatalytic and electrocatalytic reactions. A series of carbon-based catalysts with various oxygen-containing groups were synthesized by hydrogen peroxide oxidation for selective catalytic reduction (SCR) of NO with NH3.MethodsThe textural properties and oxygen-containing groups types were measured by N2adsorption-desorption and spectroscopic characterization, respectively. Denitrification experiment results show the denitrification efficiency is correlated with the oxygen contents. The density functional theory (DFT) calculations demonstrate that oxygen-containing groups can promote the chemisorption for NO and NH3, thus resulting in high performance for NO reduction.Significant findingsThe carboxyl and phenol groups on carbon materials facilitate the catalytic performance of denitrification. Furthermore, based on mechanism analysis that the formation of CO (NH4) and C(NO) on surface oxides is considered significant steps for NO reduction with NH3. Our finding paves a new strategy for the design and synthesis of SCR catalysts with excellent activity for oxygen-containing carbon material at a relatively low temperature.
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