Parallelized Screening of Characterized and DFT-Modeled Bimetallic Colloidal Cocatalysts for Photocatalytic Hydrogen Evolution
Parallelized Screening of Characterized and DFT-Modeled Bimetallic Colloidal Cocatalysts for Photocatalytic Hydrogen Evolution
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DOI：
10.1021/acscatal.9b05404
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发表时间：
2020-04-03
期刊：
影响因子：
12.9
通讯作者：
Bernhard, Stefan
中科院分区：
文献类型：
--
作者：
Lopato, Eric M.;Eikey, Emily A.;Bernhard, Stefan
采用新设计开发的并行光反应器和比色检测方法，对用于光催化减水的双金属助催化剂（Pd/Sn、Pd/Mo、Pd/Ru、Pd/Pb、Pd/Ni、Ni/Sn、Mo/Sn和Pt/Sn）进行了大样品测试。在这些助催化剂中，钯和锡的组合在钯相对含量较低的情况下表现出最高的协同行为和峰值氢气产量。对所得钯/锡双金属助催化剂进行了表征，具体而言，扫描透射电子显微镜能量色散 X 射线光谱表明钯和锡元素驻留在同一颗粒内。将钯/锡混合物的实验催化活性与密度泛函理论导出的与氢吸附到表面上相关的能量值进行比较。该比较表明，在电化学 Sabatier 火山图中发现的 Delta G(H)* = 类似于 0 eV 处的典型峰值在实验光催化系统中得到了复制，并在 Delta G(H)* = -0.036 eV 处观察到了峰值活性。此处表达的结果的计算确认证明了并行比色检测氢的功效，并提出了用于日益快速的催化剂筛选的模型。
Using a newly designed and developed parallelized photoreactor and colorimetric detection method, a large sampling of bimetallic cocatalysts (Pd/Sn, Pd/Mo, Pd/Ru, Pd/Pb, Pd/Ni, Ni/Sn, Mo/Sn, and Pt/Sn) for photocatalytic water reduction have been tested. Of these cocatalysts, the combination of palladium and tin showed the highest synergistic behavior and peak hydrogen gas production at a low relative fraction of palladium. The resulting palladium/tin bimetallic cocatalysts were characterized, and specifically, and scanning transmission electron microscopy energy-dispersive X-ray spectroscopy indicated that palladium and tin elements reside within the same particle. The experimental catalytic activity for the palladium/tin mixture was compared to density functional theory-derived energy values associated with the adsorption of hydrogen onto a surface. This comparison demonstrated that the typical peak found in electrochemical Sabatier volcano plots at Delta G(H)* = similar to 0 eV were replicated in the experimental photocatalytic system with a peak activity observed at Delta G(H)* = -0.036 eV. Computational confirmation of the results expressed here demonstrates the efficacy of colorimetric detection of hydrogen in parallel and presents a model for increasingly rapid catalyst screening.