State Key Joint Laboratory of Environment Simulation and Pollution Control, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China.
University of Chinese Academy of Sciences, Beijing 100049, China.
Environ Sci Technol. 2022 Aug 2;56(15):10916-10924. doi: 10.1021/acs.est.2c01278. Epub 2022 Jun 30.
Pt/AlO catalysts showing excellent activity and stability have been used in various reactions, including HCHO oxidation. Herein, we prepared Pt-Na/AlO catalysts with a Pt content of 0.05 wt % to reveal the key factors determining the anchoring of Pt as well as the catalytic activity and mechanism of HCHO oxidation. Pt-Na/nano-AlO (denoted as Pt-Na/nAlO) catalysts with 0.05 wt % Pt content could completely oxidize HCHO to CO at room temperature, which is the lowest Pt content used in HCHO catalytic oxidation to our knowledge. After Na addition, terminal hydroxyl groups (denoted as HO-μ) on nano-AlO were transformed to doubly bridging hydroxyl groups between Na and Al (denoted as HO-μ), which atomically dispersed Pt species. Pt anchoring further promoted the regeneration of HO-μ by activating O and HO, oxidizing HCHO to CO directly by the fast reaction step ([HCOO] + [OH] → CO + HO). Our study revealed that the HO-μ synergistically generated by HO-μ and Na species provided anchoring sites for Pt species.
具有优异活性和稳定性的 Pt/AlO 催化剂已被用于各种反应，包括 HCHO 氧化。在此，我们制备了 Pt-Na/AlO 催化剂，Pt 含量为 0.05wt%，以揭示决定 Pt 锚定的关键因素以及 HCHO 氧化的催化活性和机理。Pt-Na/nano-AlO（记为 Pt-Na/nAlO）催化剂在室温下可完全将 HCHO 氧化为 CO，这是我们所知的用于 HCHO 催化氧化的最低 Pt 含量。添加 Na 后，nano-AlO 上的末端羟基（记为 HO-μ）转变为 Na 和 Al 之间的双桥羟基（记为 HO-μ），从而原子分散 Pt 物种。Pt 锚定进一步通过激活 O 和 HO 促进了 HO-μ的再生，通过快速反应步骤（[HCOO] + [OH] → CO + HO）直接将 HCHO 氧化为 CO。我们的研究表明，HO-μ 和 Na 物种协同产生的 HO-μ 为 Pt 物种提供了锚定位点。
