论文标题

无电敏感的无电极和无共催化剂检测纳米尔盐的氢进化,以发现新的光催化剂

Ultrasensitive electrode-free and co-catalyst-free detection of nanomoles per hour hydrogen evolution for the discovery of new photocatalysts

论文作者

Huaiyu, Wang, Katz, Rebecca, Fanghanel, Julian, Schaak, Raymond E., Gopalan, Venkatraman

论文摘要

高通量理论方法越来越多地用于识别有望从水中产生氢作为清洁能源的有希望的光催化材料。虽然最有前途的水分分割候选者需要共同催化剂加载和电偏置,但预测它们的计算成本变得很大。因此,重要的是要确定具有较小初始氢生产速率的裸露的,无偏的半导体光催化剂,通常在每小时数十亿个纳米摩尔的范围内,因为随着进一步的共催化剂的加载和偏见,它们可能会变得高效。在这里,我们报告了一个敏感的氢检测系统,适合筛选新的光催化剂。检测到带有0.3%WT PT的原型金红石TIO2的氢进化速率为78.0+-0.8μmol/h/0.04G,与文献中报道的速率相当。相比之下,对于裸露的多晶TiO2,证明了对11.4+-0.3 nmol/h/0.04g的超低演化速率的敏感性。证明了两个候选光催化剂,即ZnFe2O4(18.1+-0.2 Nmol/h/0.04g)和Ca2pbo4(35.6+-0.5 nmol/h/0.04G),没有电气偏置或同源偏置负载,证明了潜在的裸露Tio2。这项工作扩展了可用于敏感检测光催化过程的技术,以更快地筛选其裸露状态

High throughput theoretical methods are increasingly used to identify promising photocatalytic materials for hydrogen generation from water as a clean source of energy. While most promising water splitting candidates require co-catalyst loading and electrical biasing, computational costs to predict them apriori becomes large. It is therefore important to identify bare, bias-free semiconductor photocatalysts with small initial hydrogen production rates, often in the range of tens of nano-mols per hour, as these can become highly efficient with further co-catalyst loading and biasing. Here we report a sensitive hydrogen detection system suitable for screening new photocatalysts. The hydrogen evolution rate of the prototypical rutile TiO2 loaded with 0.3 % wt Pt is detected to be 78.0+-0.8 μmol/h/0.04g, comparable with the rates reported in the literature. In contrast, sensitivity to an ultralow evolution rate of 11.4+-0.3 nmol/h/0.04g is demonstrated for bare polycrystalline TiO2 without electrical bias. Two candidate photocatalysts, ZnFe2O4 (18.1+-0.2 nmol/h/0.04g) and Ca2PbO4 (35.6+-0.5 nmol/h/0.04g), without electrical bias or co-catalyst loading, are demonstrated to be potentially superior to bare TiO2. This work expands the techniques available for sensitive detection of photocatalytic processes towards much faster screening of new candidate photocatalytic materials in their bare state

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