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钛改性凹凸棒石的耐碱 NO 催化还原的自卫效应。

Self-Defense Effects of Ti-Modified Attapulgite for Alkali-Resistant NO Catalytic Reduction.

机构信息

International Joint Laboratory of Catalytic Chemistry, College of Sciences, Shanghai University, Shanghai 200444, China.

出版信息

Environ Sci Technol. 2022 Apr 5;56(7):4386-4395. doi: 10.1021/acs.est.1c07996. Epub 2022 Mar 9.

Abstract

Nowadays, the serious deactivation of deNO catalysts caused by alkali metal poisoning was still a huge bottleneck in the practical application of selective catalytic reduction of NO with NH. Herein, alkali-resistant NO catalytic reduction over metal oxide catalysts using Ti-modified attapulgite (ATP) as supports has been originally demonstrated. The self-defense effects of Ti-modified ATP for alkali-resistant NO catalytic reduction have been clarified. Ti-modified ATP with self-defense ability was obtained by removing alkaline metal cation impurities in the natural ATP materials without destroying its initial layered-chain structure through the ion-exchange procedure, accompanied with an obvious enrichment of Brønsted acid and Lewis acid sites. The self-defense effects embodied that both ion-exchanged Ti octahedral centers and abundant Si-OH sites in the Ti-ion-exchange-modified ATP could effectively anchor alkali metals via coordinate bonding or ion-exchange process, which induced alkali metals to be immobilized by the Ti-ion-exchange-modified ATP carrier rather than impair active species. Under this special protection of self-defense effects, Ti-ion-exchange-modified ATP supported catalysts still retained plentiful acidic sites and superior redox ability even after alkali metal poisoning, giving rise to the maintenance of sufficient NH and NO adsorption and the subsequent efficient reaction, which in turn resulted in high NO catalytic reduction capacity of the catalyst. The strategy provided new inspiration for the development of novel and efficient selective catalytic reduction of NO with NH (NH-SCR) catalysts with high alkali resistance.

摘要

如今,碱金属中毒导致的脱硝催化剂严重失活仍然是 NH3 选择性催化还原(SCR)脱硝技术实际应用的巨大瓶颈。本文首次提出了以钛改性凹凸棒石(ATP)为载体的耐碱金属氧化物催化剂用于耐碱金属的 NO 催化还原。阐明了 Ti 改性 ATP 耐碱金属 NO 催化还原的自防御作用。通过离子交换过程,在不破坏其初始层状链结构的情况下,从天然 ATP 材料中去除碱金属阳离子杂质,获得具有自防御能力的 Ti 改性 ATP,同时明显富集了 Brønsted 酸和 Lewis 酸位。自防御作用体现在 Ti 离子交换改性 ATP 中的离子交换 Ti 八面体中心和丰富的 Si-OH 位可以通过配位键或离子交换过程有效地固定碱金属,从而导致碱金属被 Ti 离子交换改性 ATP 载体固定,而不是破坏活性物种。在这种特殊的自防御作用的保护下,Ti 离子交换改性 ATP 负载催化剂即使在碱金属中毒后仍保留大量的酸性位和优异的氧化还原能力,从而保持足够的 NH 和 NO 吸附和随后的高效反应,进而导致催化剂具有高的 NO 催化还原能力。该策略为开发具有高耐碱金属性能的新型高效 NH3 选择性催化还原(NH-SCR)催化剂提供了新的思路。

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