Issue 15, 2024

Nanostructured hybrid catalysts empower the artificial leaf for solar-driven ammonia production from nitrate

Abstract

Converting solar energy into chemicals and fuels through photoelectrocatalytic (PEC) process is challenging but holds significant potential for advancing sustainable development. Here we introduce an innovative system to realize solar-driven NH3 production from waste nitrate by nano-structured top layer (NSTL) hybrid catalysts modified commercial Si absorber, to bridge the gap from fundamental understanding to the process engineering. Specifically, we employ a rationally designed Si/Cu-NSTL/Co(OH)2 ternary photocathode featuring a Schottky barrier contact enabling optimized photo-carrier transport pathways and a beneficial co-adsorption configuration of *NO3–H2O moieties. This photocathode exhibits the best-known performance in the literature for the PEC conversion of NO3 to NH3, boasting an onset potential of approximately 1 VRHE and a remarkable faradaic efficiency of nearly 100%. Building upon these findings, we develop the first large-scale unbiased PEC device (an artificial leaf) capable of simultaneously producing NH3 and valorizing biomass, achieving a solar utilization efficiency of approximately 4%. Its scalability and practical feasibility have been further validated through rigorous outdoor testing with an assembled tandem device array. The process techno-economic assessment shows compelling economic viability of this technology across diverse application scenarios in NH3 production, resulting in substantial savings of fossil fuel and a reduction of CO2 emissions. We anticipate that this work will serve as a valuable resource for the design of next-generation photoelectrodes and devices, bringing us one step closer to realizing standalone solar-to-sustainable chemical applications.

Graphical abstract: Nanostructured hybrid catalysts empower the artificial leaf for solar-driven ammonia production from nitrate

Supplementary files

Article information

Article type
Paper
Submitted
09 Nov 2023
Accepted
01 Jul 2024
First published
02 Jul 2024

Energy Environ. Sci., 2024,17, 5653-5665

Nanostructured hybrid catalysts empower the artificial leaf for solar-driven ammonia production from nitrate

C. Han, C. Li, J. A. Yuwono, Z. Liu, K. Sun, K. Wang, G. He, J. Huang, P. V. Kumar, J. Vongsvivut, J. Cong, H. Mehrvarz, Z. Han, X. Lu, J. Pan, X. Hao and R. Amal, Energy Environ. Sci., 2024, 17, 5653 DOI: 10.1039/D3EE03836J

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