Engineering a Kesterite-Based Photocathode for Photoelectrochemical Ammonia Synthesis from NOx Reduction

Engineering a Kesterite-Based Photocathode for Photoelectrochemical Ammonia Synthesis from NOx Reduction

© 2022 The Authors. Advanced Materials published by Wiley-VCH GmbH.

Détails bibliographiques
Publié dans:Advanced materials (Deerfield Beach, Fla.). - 1998. - 34(2022), 29 vom: 01. Juli, Seite e2201670
Auteur principal: Zhou, Shujie (Auteur)
Autres auteurs: Sun, Kaiwen, Toe, Cui Ying, Yin, Jun, Huang, Jialiang, Zeng, Yiyu, Zhang, Doudou, Chen, Weijian, Mohammed, Omar F, Hao, Xiaojing, Amal, Rose
Format: Article en ligne
Langue:English
Publié: 2022
Accès à la collection:Advanced materials (Deerfield Beach, Fla.)
Sujets:Journal Article NOx reduction TiOx ammonia synthesis defect engineering kesterite photocathodes
Description
Résumé:© 2022 The Authors. Advanced Materials published by Wiley-VCH GmbH.
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 (NOx RR) 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 NOx RR by a kesterite (Cu2 ZnSnS4 [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 NOx RR, 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
Description:Date Revised 21.07.2022
published: Print-Electronic
Citation Status PubMed-not-MEDLINE
ISSN:1521-4095
DOI:10.1002/adma.202201670