Department of Chemistry, Michigan State University , 578 S Shaw Lane, East Lansing, Michigan 48824-1322, United States.
Langmuir. 2017 Oct 17;33(41):10800-10806. doi: 10.1021/acs.langmuir.7b02414. Epub 2017 Oct 4.
Thin films of TaOH were cathodically electrodeposited from an aqueous solution containing Ta-IPA precursor and KNO as a sacrificial agent. It was shown that the deposition resulted from a precipitation reaction triggered by the local change of pH at the surface of working electrode. Combined structural and compositional analysis revealed that during the electrodeposition the oxidation state of tantalum remained constant, Ta(V). The as-deposited films are mesoporous amorphous tantalum oxide hydrate films, which can be converted to either pure TaO or TaN by high-temperature annealing in either air (or Ar) or ammonia, respectively. The TaN electrodes exhibited promising PEC activity for water oxidation. These results open the door for the reduced temperature synthesis of TaN electrodes on TCO substrates which would allow for efficient overall solar water splitting.
TaOH 薄膜通过在含有 Ta-IPA 前体和 KNO 作为牺牲剂的水溶液中阴极电沉积而获得。结果表明，沉积是由工作电极表面局部 pH 值变化引发的沉淀反应引起的。结构和组成分析表明，在电沉积过程中，钽的氧化态保持不变，为 Ta(V)。所得的薄膜是介孔无定形氧化钽水合物薄膜，通过在空气（或 Ar）或氨中分别进行高温退火，可分别转化为纯 TaO 或 TaN。TaN 电极表现出用于水氧化的有前景的 PEC 活性。这些结果为在 TCO 衬底上低温合成 TaN 电极开辟了道路，这将允许有效进行整体太阳能水分解。
