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协同催化去除 NO 和正丁胺通过空间分离的协同位点。

Synergistic Catalytic Removal of NO and -Butylamine via Spatially Separated Cooperative Sites.

机构信息

School of Environmental and Chemical Engineering, State Key Laboratory of Advanced Special Steel, International Joint Laboratory of Catalytic Chemistry, Innovation Institute of Carbon Neutrality, College of Sciences, Shanghai University, Shanghai 200444, China.

出版信息

Environ Sci Technol. 2024 Jul 2;58(26):11781-11790. doi: 10.1021/acs.est.4c01840. Epub 2024 Jun 15.

DOI:10.1021/acs.est.4c01840
PMID:38877971
Abstract

Synergistic control of nitrogen oxides (NO) and nitrogen-containing volatile organic compounds (NVOCs) from industrial furnaces is necessary. Generally, the elimination of -butylamine (-B), a typical pollutant of NVOCs, requires a catalyst with sufficient redox ability. This process induces the production of nitrogen-containing byproducts (NO, NO, NO), leading to lower N selectivity of NH selective catalytic reduction of NO (NH-SCR). Here, synergistic catalytic removal of NO and -B via spatially separated cooperative sites was originally demonstrated. Specifically, titania nanotubes supported CuO-CeO (CuCe-TiO NTs) catalysts with spatially separated cooperative sites were creatively developed, which showed a broader active temperature window from 180 to 340 °C, with over 90% NO conversion, 85% -B conversion, and 90% N selectivity. A synergistic effect of the Cu and Ce sites was found. The catalytic oxidation of -B mainly occurred at the Cu sites inside the tube, which ensured the regular occurrence of the NH-SCR reaction on the outer Ce sites under the matching temperature window. In addition, the -B oxidation would produce abundant intermediate NH*, which could act as an extra reductant to promote NH-SCR. Meanwhile, NH-SCR could simultaneously remove the possible NO byproducts of -B decomposition. This novel strategy of constructing cooperative sites provides a distinct pathway for promoting the synergistic removal of -B and NO.

摘要

协同控制工业炉中的氮氧化物 (NO) 和含氮挥发性有机化合物 (NVOCs) 是必要的。通常,消除 - 丁胺 (-B),一种典型的 NVOCs 污染物,需要具有足够氧化还原能力的催化剂。该过程会诱导含氮副产物(NO、NO、NO)的产生,从而降低 NH 选择性催化还原 NO(NH-SCR)的 N 选择性。本文首次提出通过空间分离的协同位协同催化去除 NO 和 -B。具体来说,创造性地开发了具有空间分离协同位的负载 CuO-CeO 的 TiO NTs(CuCe-TiO NTs)催化剂,其具有从 180 到 340°C 的更宽的活性温度窗口,NO 转化率超过 90%,-B 转化率超过 85%,N 选择性超过 90%。发现 Cu 和 Ce 位之间存在协同效应。-B 的催化氧化主要发生在管内的 Cu 位,这确保了在匹配的温度窗口下,NH-SCR 反应在管外的 Ce 位上正常进行。此外,-B 氧化会产生丰富的中间 NH*,它可以作为额外的还原剂来促进 NH-SCR。同时,NH-SCR 可以同时去除 -B 分解可能产生的 NO 副产物。这种构建协同位的新策略为促进 -B 和 NO 的协同去除提供了一条明显的途径。

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