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On the Role of Sn Segregation of Pt-Sn Catalysts for Propane Dehydrogenation
ACS Catalysis ( IF 11.3 ) Pub Date : 2021-03-25 , DOI: 10.1021/acscatal.1c00639 Jieli Wang 1, 2 , Xin Chang 1, 2 , Sai Chen 1, 2 , Guodong Sun 1, 2 , Xiaohong Zhou 3 , Evgeny Vovk 3 , Yong Yang 3 , Wanyu Deng 1, 2 , Zhi-Jian Zhao 1, 2 , Rentao Mu 1, 2 , Chunlei Pei 1, 2 , Jinlong Gong 1, 2, 4
ACS Catalysis ( IF 11.3 ) Pub Date : 2021-03-25 , DOI: 10.1021/acscatal.1c00639 Jieli Wang 1, 2 , Xin Chang 1, 2 , Sai Chen 1, 2 , Guodong Sun 1, 2 , Xiaohong Zhou 3 , Evgeny Vovk 3 , Yong Yang 3 , Wanyu Deng 1, 2 , Zhi-Jian Zhao 1, 2 , Rentao Mu 1, 2 , Chunlei Pei 1, 2 , Jinlong Gong 1, 2, 4
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Bimetallic nanoparticle catalysts attract extensive attention for relevant catalysis processes due to their flexible structures, while the structure evolution under specific conditions is ambiguous. This paper describes the structure evolution of Pt-Sn bimetallic nanoparticles for catalytic dehydrogenation, especially Sn segregation for surface recovery of a Pt-Sn alloy. An acid etching-reduction process was adopted to investigate the migration of Sn atoms after surface Sn species loss. By acid etching, Sn atoms at the surface of Pt-Sn alloy nanoparticles were removed, leaving nanoparticles with a Pt-rich shell and an unchanged Pt3Sn alloy core. Excitedly, during the following reduction process, the Pt3Sn alloy surface was recovered due to the migration of Sn atoms from the core to the surface, as confirmed by transmission electron microscopy, quasi in situ X-ray photoelectron spectroscopy, and density functional theory calculations. Subsequent studies on the catalyst performance for propane dehydrogenation (PDH) showed that the recoverable Pt3Sn alloy surface structure contributed to the high efficiency with 92% propene selectivity even after 5 cycles of the acid etching-reduction procedure. The recovery of the Pt-Sn alloy through Sn segregation could enable catalysts to overcome component fluctuations, making an efficient catalytic process.
中文翻译：
Pt-Sn催化剂中Sn的离析对丙烷脱氢的作用
双金属纳米颗粒催化剂由于其柔性结构而在相关的催化过程中引起了广泛的关注，而在特定条件下的结构演变却是模棱两可的。本文描述了用于催化脱氢的Pt-Sn双金属纳米粒子的结构演变，特别是用于Pt-Sn合金表面恢复的Sn偏析。采用酸腐蚀还原工艺研究了表面Sn物种流失后Sn原子的迁移。通过酸蚀刻，去除了Pt-Sn合金纳米颗粒表面的Sn原子，从而使纳米颗粒具有富Pt的壳层和不变的Pt 3 Sn合金核。令人兴奋的是，在接下来的还原过程中，Pt 3如透射电子显微镜，准原位X射线光电子能谱和密度泛函理论计算所证实的，由于锡原子从核向表面的迁移，锡合金表面得以恢复。随后对丙烷脱氢（PDH）催化剂性能的研究表明，即使经过5次酸蚀-还原过程，可回收的Pt 3 Sn合金表面结构也能以92％的丙烯选择性提高效率。通过Sn偏析回收Pt-Sn合金可以使催化剂克服组分波动，从而实现高效的催化过程。
更新日期：2021-04-16
中文翻译：
Pt-Sn催化剂中Sn的离析对丙烷脱氢的作用
双金属纳米颗粒催化剂由于其柔性结构而在相关的催化过程中引起了广泛的关注，而在特定条件下的结构演变却是模棱两可的。本文描述了用于催化脱氢的Pt-Sn双金属纳米粒子的结构演变，特别是用于Pt-Sn合金表面恢复的Sn偏析。采用酸腐蚀还原工艺研究了表面Sn物种流失后Sn原子的迁移。通过酸蚀刻，去除了Pt-Sn合金纳米颗粒表面的Sn原子，从而使纳米颗粒具有富Pt的壳层和不变的Pt 3 Sn合金核。令人兴奋的是，在接下来的还原过程中，Pt 3如透射电子显微镜，准原位X射线光电子能谱和密度泛函理论计算所证实的，由于锡原子从核向表面的迁移，锡合金表面得以恢复。随后对丙烷脱氢（PDH）催化剂性能的研究表明，即使经过5次酸蚀-还原过程，可回收的Pt 3 Sn合金表面结构也能以92％的丙烯选择性提高效率。通过Sn偏析回收Pt-Sn合金可以使催化剂克服组分波动，从而实现高效的催化过程。
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