Atmospheric nitrogen fixation using a photocatalytic system is a promising approach to produce ammonia. However, most of the recently explored photocatalysts for N 2 fixation are in the powder form, suffering from agglomeration and difficulty in the collection and leading to unsatisfactory conversion efficiency. Developing efficient film catalysts for N 2 photofixation under ambient conditions remains challenging. Herein, we report the efficient photofixation of N 2 over a periodic WS 2 @TiO 2 nanoporous film, which is fabricated through a facile method that combines anodization, E-beam evaporation, and chemical vapor deposition (CVD). Oxygen vacancies are introduced into TiO 2 nanoporous films through Ar annealing treatment, which plays a vital role in N 2 adsorption and activation. The periodic WS 2 @TiO 2 nanoporous film with an optimized WS 2 content shows highly efficient photocatalytic performance for N 2 fixation with an NH 3 evolution rate of 1.39 mmol g −1 h −1 , representing one of the state-of-the-art catalysts.
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Ultrasensitive electrode-free and co-catalyst-free detection of nanomoles per hour hydrogen evolution for the discovery of new photocatalysts
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 a priori become 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 nanomoles 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 TiO 2 loaded with 0.3 wt. % Pt is detected to be 78.0 ± 0.8 µmol/h/0.04 g, comparable with the rates reported in the literature. In contrast, sensitivity to an ultralow evolution rate of 11.4 ± 0.3 nmol/h/0.04 g is demonstrated for bare polycrystalline TiO 2 without electrical bias. Two candidate photocatalysts, ZnFe 2 O 4 (18.1 ± 0.2 nmol/h/0.04 g) and Ca 2 PbO 4 (35.6 ± 0.5 nmol/h/0.04 g) without electrical bias or co-catalyst loading, are demonstrated to be potentially superior to bare TiO 2 . This work expands the techniques available for sensitive detection of photocatalytic processes toward much faster screening of new candidate photocatalytic materials in their bare state.
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- Award ID(s):
- 1729338
- PAR ID:
- 10401096
- Date Published:
- Journal Name:
- Review of Scientific Instruments
- Volume:
- 93
- Issue:
- 2
- ISSN:
- 0034-6748
- Page Range / eLocation ID:
- 025002
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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