- Title
- Engineering a Kesterite-Based Photocathode for Photoelectrochemical Ammonia Synthesis from NO
x Reduction - Creator
- Zhou, Shujie; Sun, Kaiwen; Amal, Rose; Toe, Cui Ying; Yin, Jun; Huang, Jialiang; Zeng, Yiyu; Zhang, Doudou; Chen, Weijian; Mohammed, Omar F.; Hao, Xiaojing
- Relation
- Advanced Materials Vol. 34, Issue 29, no. 2201670
- Publisher Link
- http://dx.doi.org/10.1002/adma.202201670
- Publisher
- Wiley-VCH Verlag GmbH & Co. KGaA
- Resource Type
- journal article
- Date
- 2022
- Description
- Ammonia is a key chemical feedstock for industry as well as future carbon-free fuel and transportable vector for renewable energy. Photoelectrochemical (PEC) ammonia synthesis from NOx reduction reaction (NOxRR) provides not only a promising alternative to the energy-intensive Haber–Bosch process through direct solar-to-ammonia conversion, but a sustainable solution for balancing the global nitrogen cycle by restoring ammonia from wastewater. In this work, selective ammonia synthesis from PEC NOxRR by a kesterite (Cu2ZnSnS4 [CZTS]) photocathode through loading defect-engineered TiOx cocatalyst on a CdS/CZTS photocathode (TiOx/CdS/CZTS) is demonstrated. The uniquely designed photocathode enables selective ammonia production from NOxRR, yielding up to 89.1% Faradaic efficiency (FE) (0.1 V vs reversible hydrogen electrode (RHE)) with a remarkable positive onset potential (0.38 V vs RHE). By tailoring the amount of surface defective Ti3+ species, the adsorption of reactant NO3− and *NO2 intermediate is significantly promoted while the full coverage of TiOx also suppresses NO2− liberation as a by-product, contributing to high ammonia selectivity. Further attempts on PEC ammonia synthesis from simulated wastewater show good FE of 64.9%, unveiling the potential of using the kesterite-based photocathode for sustainably restoring ammonia from nitrate-rich wastewater.
- Subject
- ammonia synthesis; defect engineering; kesterite photocathodes; NOx reduction; TiOx; SDG 6; SDG 7; SDG 9; Sustainable Development Goals
- Identifier
- http://hdl.handle.net/1959.13/1483661
- Identifier
- uon:51158
- Identifier
- ISSN:0935-9648
- Language
- eng
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