{"title":"Brush-Like Hollow PtTe2 Nanotube for Enhanced Formic Acid Electrooxidation Catalysis","authors":"Qiaorong Jiang, Zhiyi Wang, Zijian Huang, Xuyuan Nie, Linzhe Lü, Xiao Han, Wei Yan, Hu Yang, Xianmeng Song, Haixin Lin, Zi-Ang Nan, Zhaoxiong Xie","doi":"10.1021/acs.jpcc.4c05900","DOIUrl":null,"url":null,"abstract":"The serious CO poisoning for traditional Pt-based catalysts often results in a large deterioration in activity and stability of formic acid oxidation reaction (FAOR), which severely restricts the development of direct formic acid fuel cells. It is of great significance and challenging to enhance the CO tolerance for an advanced Pt-based catalyst. Whereupon, in this work, successful synthesis of a brush-like hierarchical structure composed by ordered ultrathin PtTe<sub>2</sub> intermetallic compounds is achieved. Benefiting from the electron transfer from Pt to Te, the relatively poor electron density of Pt can assist the down shift of the d-band center of PtTe<sub>2</sub>, which greatly weakens the adsorption affinity toward CO and enhances the antipoisoning ability. Besides, in situ infrared spectroscopy and density functional theory simulation further confirm the special electron structure can promote the dehydrogenation pathway during the whole FAOR proceeding. Specifically, the mass activity of PtTe<sub>2</sub> is up to 4.72 A mg<sub>pt</sub><sup>–1</sup>, which is about 9.25-fold higher than that of the commercial Pt/C. In addition, PtTe<sub>2</sub> still has higher catalytic activity than commercial Pt/C even after 3 h. This work inspires targeted enhancement of the antipoisoning properties of Pt-based catalysts through the design of atomic level ordered structure and ultrathin two-dimensional morphology and is beneficial to the considerable progress of fuel cell catalysis.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"17 1","pages":""},"PeriodicalIF":3.3000,"publicationDate":"2024-11-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"The Journal of Physical Chemistry C","FirstCategoryId":"1","ListUrlMain":"https://doi.org/10.1021/acs.jpcc.4c05900","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
Abstract
The serious CO poisoning for traditional Pt-based catalysts often results in a large deterioration in activity and stability of formic acid oxidation reaction (FAOR), which severely restricts the development of direct formic acid fuel cells. It is of great significance and challenging to enhance the CO tolerance for an advanced Pt-based catalyst. Whereupon, in this work, successful synthesis of a brush-like hierarchical structure composed by ordered ultrathin PtTe2 intermetallic compounds is achieved. Benefiting from the electron transfer from Pt to Te, the relatively poor electron density of Pt can assist the down shift of the d-band center of PtTe2, which greatly weakens the adsorption affinity toward CO and enhances the antipoisoning ability. Besides, in situ infrared spectroscopy and density functional theory simulation further confirm the special electron structure can promote the dehydrogenation pathway during the whole FAOR proceeding. Specifically, the mass activity of PtTe2 is up to 4.72 A mgpt–1, which is about 9.25-fold higher than that of the commercial Pt/C. In addition, PtTe2 still has higher catalytic activity than commercial Pt/C even after 3 h. This work inspires targeted enhancement of the antipoisoning properties of Pt-based catalysts through the design of atomic level ordered structure and ultrathin two-dimensional morphology and is beneficial to the considerable progress of fuel cell catalysis.
传统pt基催化剂严重的CO中毒往往导致甲酸氧化反应(FAOR)的活性和稳定性大幅下降,严重制约了直接甲酸燃料电池的发展。提高高级pt基催化剂的CO耐受性具有重要的意义和挑战性。因此,在这项工作中,成功地合成了由有序超薄PtTe2金属间化合物组成的刷状分层结构。Pt相对较低的电子密度受益于Pt向Te的电子转移,有助于PtTe2的d带中心下移,从而大大削弱了PtTe2对CO的吸附亲和力,增强了其抗中毒能力。此外,原位红外光谱和密度泛函理论模拟进一步证实了特殊的电子结构可以促进整个FAOR过程中的脱氢途径。具体而言,PtTe2的质量活性高达4.72 A mgpt-1,比商用Pt/C高约9.25倍。此外,即使在3 h后,PtTe2仍具有比商用Pt/C更高的催化活性。本工作通过原子级有序结构和超薄二维形态的设计,激发了Pt基催化剂的抗中毒性能的针对性增强,有利于燃料电池催化的长足发展。
期刊介绍:
The Journal of Physical Chemistry A/B/C is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, and chemical physicists.