4.8 Article

Photocatalytic NH3 versus H2 evolution over g-C3N4/CsxWO3: O2 and methanol tipping the scale

Journal

APPLIED CATALYSIS B-ENVIRONMENTAL
Volume 235, Issue -, Pages 197-206

Publisher

ELSEVIER SCIENCE BV
DOI: 10.1016/j.apcatb.2018.04.081

Keywords

Photocatalysis; N-2 fixation; H-2 evolution; O-2 content; Sacrificial agent

Funding

  1. National Natural Science Foundation of China [51402139]
  2. JSPS KAKENHI Grant [JP16H06439]
  3. Dynamic Alliance for Open Innovation Bridging Human, Environment and Materials
  4. Cooperative Research Program of Network Joint Research Center for Materials and Devices

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CsxWO3 nanorods can be used to sensitize the single layer g-C3N4, where full spectrum light harvesting excited electrons to drive the photocatalytic reduction of N-2 into NH3. Under UV light, both water splitting and solar ammonia synthesis reaction exhibit high activity. However, selectivity towards ammonia over hydrogen is realized under NIR irradiation. With the control of methanol, O-2 can directly decide the NH3 or H-2 evolution on photocatalyst. The origin is the strong capture of O-2 with the electrons from the photocatalyst under light irradiation to yield the oxygen active species, which transfer electrons subsequently with help of methanol to generate NH3. However, H-2 production will be suppressed by O-2. And with its sacrifice, methanol preserves the produced NH3 from oxidation. The O-2-sacrificial agent mediated NH3 evolution reaction found here provides insights in the promotion role of them in other catalysis.

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