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碳原子掺杂的铂活性位点实现了乙烯在低温下的高活性和稳定催化氧化。

Carbon Atom Doped Pt Active Sites Enable Highly Active and Stable Catalytic Oxidation of Ethylene at Low Temperatures.

作者信息

Zhao Qian, Lu Xuxing, Fu Heyun, Qu Xiaolei, Zheng Shourong, Zhu Dongqiang

机构信息

State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing 210023, China.

School of Urban and Environmental Sciences, Peking University, Beijing 100871, China.

出版信息

Environ Sci Technol. 2025 Jul 1;59(25):13042-13053. doi: 10.1021/acs.est.4c14721. Epub 2025 Jun 13.

Abstract

Precisely tuning the surface properties of Pt active sites is of great importance for designing highly active catalysts used in the low-temperature catalytic oxidation of ethylene (CH). Herein, carbon doped Pt catalysts supported on SBA-15 (PtC/SBA-15) were prepared by ethane (CH) heat treatment on SBA-15 supported Pt catalysts (Pt/SBA-15). Characterization results disclose that carbon atoms are successfully introduced in Pt particles, forming unique PtC active sites. The PtC active sites exhibit strong CH adsorption and activation ability, enhanced hydrophobicity, and high catalytic activity for CO oxidation. As a result, PtC/SBA-15 catalysts exhibit much higher CH conversion and CO yield than Pt/SBA-15 catalysts at 0 °C. Particularly, 3PtC/SBA-15 maintains 100% conversion of 50 ppm of CH for more than 7 h and even displays 93.2% CH conversion and 88.8% CO yield after 20 h of time-on-stream (TOS), exhibiting unprecedentedly prominent catalytic performance. This study provides a universal and efficient strategy to accurately enhance the surface hydrophobicity of noble metal particles employed in the low-temperature catalytic oxidation of CH. More importantly, it opens a new pathway for constructing highly active catalysts from the perspective of accelerating the oxidation of intermediate species to achieve improved utilization efficiency of active sites.

摘要

精确调控铂活性位点的表面性质对于设计用于乙烯(CH)低温催化氧化的高活性催化剂至关重要。在此,通过对SBA-15负载的铂催化剂(Pt/SBA-15)进行乙烷(CH)热处理,制备了SBA-15负载的碳掺杂铂催化剂(PtC/SBA-15)。表征结果表明,碳原子成功引入到铂颗粒中,形成了独特的PtC活性位点。PtC活性位点表现出较强的CH吸附和活化能力、增强的疏水性以及对CO氧化的高催化活性。因此,在0°C时,PtC/SBA-15催化剂比Pt/SBA-15催化剂表现出更高的CH转化率和CO产率。特别是,3PtC/SBA-15在超过7小时内保持50 ppm CH的100%转化率,甚至在连续运行(TOS)20小时后仍显示出93.2%的CH转化率和88.8%的CO产率,展现出前所未有的卓越催化性能。本研究提供了一种通用且高效的策略,以精确增强用于CH低温催化氧化的贵金属颗粒的表面疏水性。更重要的是,它从加速中间物种氧化以提高活性位点利用效率的角度,为构建高活性催化剂开辟了一条新途径。

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