Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2023-10-15 , DOI: 10.1016/j.cej.2023.146709 Haiyin Zhong , Ruixuan Wang , Zhihao Yan , Li Ling , Hong Li
Understanding the details of how Pt-O/Pt active sites are boosted is essential for many catalytic reactions. Herein, different anatase/rutile (A/R) phase ratios of TiO2 nanoparticles (NPs) prepared by controlling calcination temperature (T), and irreversibly adsorbed Bi(III) are employed to dually improve the Pt-O/Pt active sites and their electrocatalytic activities. It is found that a T-dependent concave improvement trend is obtained on Pt/TiO2-T for the Pt-O/Pt active sites and electrocatalytic methanol oxidation rate. In the simultaneous presence of TiO2-T and BiOx, the electron-rich R(1 1 0) facet of TiO2-950 can promote the formation of bimetallic Bi-Pt sites, and the oxygen-acceptable Bi(III) is favorite for the electrochemical assembly of {Bi-Ox-Pt} active sites on the R(1 1 0) facet, further achieving a remarkable increase of 19.7-fold and 4.5-fold for the Pt-O/Pt active sites and electrocatalytic activity towards methanol oxidation compared with the case of bare Pt electrodes, respectively. The relationship between the Pt-O/Pt active sites and electrocatalytic properties is demonstrated, and the complete oxidation mechanism of methanol is proposed on BiOx-[Pt-TiO2-950] with reliable long-term durability. This study shows a new dually tuning strategy to maximize the utilization efficiency and anti-deactivated ability of Pt-based catalysts by TiO2-T and BiOx.
中文翻译:
锐钛矿/金红石 TiO2 和 BiOx 双重增强了 Pt-O/Pt 甲醇氧化活性位点和电催化性能
了解 Pt-O/Pt 活性位点如何增强的细节对于许多催化反应至关重要。在此,通过控制煅烧温度(T )制备的TiO 2纳米颗粒(NPs )的不同锐钛矿/金红石(A/R)相比和不可逆吸附的Bi(III)被用于双重改善Pt-O/Pt活性位点和它们的电催化活性。结果发现, Pt/TiO 2 - T的Pt-O/Pt活性位点和电催化甲醇氧化速率均呈现出依赖于T的凹改善趋势。在TiO 2 - T和BiO x同时存在的情况下,TiO 2 -950的富电子R(1 1 0)面可以促进双金属Bi-Pt位点的形成,氧可接受的Bi(III)为最适合在 R(1 1 0) 面上电化学组装 {Bi-O x -Pt}活性位点,进一步实现 Pt-O/Pt 活性位点和电催化性能分别显着增加 19.7 倍和 4.5 倍分别与裸 Pt 电极的情况相比,对甲醇氧化的活性。论证了Pt-O/Pt活性位点与电催化性能之间的关系,并提出了在BiO x -[Pt-TiO 2 -950]上甲醇的完全氧化机理,具有可靠的长期耐久性。本研究提出了一种新的双重调节策略,可最大限度地提高TiO 2 - T和BiO x铂基催化剂的利用率和抗失活能力。