He Limin, Wang Yangdong, Gao Huanxin, Liu Zhicheng, Xie Zaiku
State Key Laboratory of Green Chemical Engineering and Industrial Catalysis, Shanghai Research Institute of Petrochemical Technology, SINOPEC Corp. Shanghai 201208 China
China Petrochemical Corporation (SINOPEC Group) Beijing 100728 China
RSC Adv. 2021 Oct 14;11(53):33646-33652. doi: 10.1039/d1ra06479g. eCollection 2021 Oct 8.
The purification of crude terephthalic acid was performed by the hydrogenation of 4-carboxybenzaldehyde (4-CBA) over activated carbon (AC) supported Pd catalysts in industry. However, traditional Pd/AC catalysts usually suffer from low hydrogenation activity and poor thermal stability. Herein, nitrogen was incorporated into AC a simple hydrothermal treatment of AC with urea as the nitrogen resource. The N doped AC contained pyridinic N, pyrrolic N, graphitic N and oxidized N. Wide characterizations revealed that N doping not only effectively improved the dispersion of Pd NPs but also increased the proportion of Pd. In addition, N doping also enhanced the dissociative adsorption capacity of molecular hydrogen. More importantly, the resistance to sintering of Pd NPs was efficiently suppressed after N doping. As a result, N doped AC supported Pd showed both higher activity and better thermal stability than the N-free one.
在工业上，粗对苯二甲酸的提纯是通过在活性炭（AC）负载的钯催化剂上对4-羧基苯甲醛（4-CBA）进行氢化来实现的。然而，传统的Pd/AC催化剂通常存在氢化活性低和热稳定性差的问题。在此，通过以尿素作为氮源对AC进行简单的水热处理，将氮引入到AC中。N掺杂的AC含有吡啶型N、吡咯型N、石墨型N和氧化型N。广泛的表征表明，N掺杂不仅有效地改善了钯纳米颗粒（Pd NPs）的分散性，还增加了Pd的比例。此外，N掺杂还增强了分子氢的解离吸附能力。更重要的是，N掺杂后有效地抑制了Pd NPs的烧结抗性。结果，N掺杂AC负载Pd比无N的催化剂表现出更高的活性和更好的热稳定性。
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