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Cascade NH3 Oxidation and N2O Decomposition via Bifunctional Co and Cu Catalysts
ACS Catalysis ( IF 11.3 ) Pub Date : 2023-10-12 , DOI: 10.1021/acscatal.3c02392 Xuze Guan 1 , Hiroyuki Asakura 2, 3 , Rong Han 4 , Siyuan Xu 4 , Hao-Xin Liu 5 , Lu Chen 1 , Zhangyi Yao 1 , Jay Hon Cheung Yan 1 , Tsunehiro Tanaka 3 , Yuzheng Guo 4 , Chun-Jiang Jia 5 , Feng Ryan Wang 1
ACS Catalysis ( IF 11.3 ) Pub Date : 2023-10-12 , DOI: 10.1021/acscatal.3c02392 Xuze Guan 1 , Hiroyuki Asakura 2, 3 , Rong Han 4 , Siyuan Xu 4 , Hao-Xin Liu 5 , Lu Chen 1 , Zhangyi Yao 1 , Jay Hon Cheung Yan 1 , Tsunehiro Tanaka 3 , Yuzheng Guo 4 , Chun-Jiang Jia 5 , Feng Ryan Wang 1
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The selective catalytic oxidation of NH3 (NH3–SCO) to N2 is an important reaction for the treatment of diesel engine exhaust. Co3O4 has the highest activity among non-noble metals but suffers from N2O release. Such N2O emissions have recently been regulated due to having a 300× higher greenhouse gas effect than CO2. Here, we design CuO-supported Co3O4 as a cascade catalyst for the selective oxidation of NH3 to N2. The NH3–SCO reaction on CuO–Co3O4 follows a de-N2O pathway. Co3O4 activates gaseous oxygen to form N2O. The high redox property of the CuO–Co3O4 interface promotes the breaking of the N–O bond in N2O to form N2. The addition of CuO–Co3O4 to the Pt–Al2O3 catalyst reduces the full NH3 conversion temperature by 50 K and improves the N2 selectivity by 20%. These findings provide a promising strategy for reducing N2O emissions and will contribute to the rational design and development of non-noble metal catalysts.
中文翻译：
通过双功能 Co 和 Cu 催化剂进行级联 NH3 氧化和 N2O 分解
NH 3 (NH 3 –SCO)选择性催化氧化为N 2是处理柴油机废气的重要反应。Co 3 O 4在非贵金属中具有最高的活性，但会释放N 2 O。这种N 2 O排放最近由于其温室气体效应比CO 2高300倍而受到管制。在这里，我们设计了CuO负载的Co 3 O 4作为级联催化剂，用于将NH 3选择性氧化为N 2。CuO-Co 3 O 4上的NH 3 –SCO 反应遵循脱N 2 O 途径。Co 3 O 4活化气态氧形成N 2 O。CuO-Co 3 O 4界面的高氧化还原性促进N 2 O中N-O键的断裂形成N 2。在Pt-Al 2 O 3催化剂中添加CuO-Co 3 O 4可使NH 3完全转化温度降低50 K，并将N 2选择性提高20%。这些发现为减少N 2 O排放提供了一种有前途的策略，并将有助于非贵金属催化剂的合理设计和开发。
更新日期：2023-10-12
中文翻译：
通过双功能 Co 和 Cu 催化剂进行级联 NH3 氧化和 N2O 分解
NH 3 (NH 3 –SCO)选择性催化氧化为N 2是处理柴油机废气的重要反应。Co 3 O 4在非贵金属中具有最高的活性，但会释放N 2 O。这种N 2 O排放最近由于其温室气体效应比CO 2高300倍而受到管制。在这里，我们设计了CuO负载的Co 3 O 4作为级联催化剂，用于将NH 3选择性氧化为N 2。CuO-Co 3 O 4上的NH 3 –SCO 反应遵循脱N 2 O 途径。Co 3 O 4活化气态氧形成N 2 O。CuO-Co 3 O 4界面的高氧化还原性促进N 2 O中N-O键的断裂形成N 2。在Pt-Al 2 O 3催化剂中添加CuO-Co 3 O 4可使NH 3完全转化温度降低50 K，并将N 2选择性提高20%。这些发现为减少N 2 O排放提供了一种有前途的策略，并将有助于非贵金属催化剂的合理设计和开发。
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