Machine Learning Boosted Entropy-Engineered Synthesis of CuCo Nanometric Solid Solution Alloys for Near-100% Nitrate-to-Ammonia Selectivity

• Main Authors: Hu, Yao, Lan, Haihui, Hu, Bo, Gong, Jiaxuan, Wang, Donghui, Zhang, Wen-Da, Yan, Mo, Xia, Huicong, Yao, Mingde, Du, Mingliang
• Format: Journal Article
• Language: English
• Published: 31-07-2024
• Subjects: Physics - Applied Physics; Physics - Materials Science
• DOI: 10.48550/arxiv.2408.00142

Nanometric solid solution alloys are utilized in a broad range of fields,
including catalysis, energy storage, medical application, and sensor
technology. Unfortunately, the synthesis of these alloys becomes increasingly
challenging as the disparity between the metal elements grows, due to
differences in atomic sizes, melting points, and chemical affinities. This
study utilized a data-driven approach incorporating sample balancing
enhancement techniques and multilayer perceptron (MLP) algorithms to improve
the model's ability to handle imbalanced data, significantly boosting the
efficiency of experimental parameter optimization. Building on this enhanced
data processing framework, we developed an entropy-engineered synthesis
approach specifically designed to produce stable, nanometric copper and cobalt
(CuCo) solid solution alloys. Under conditions of -0.425 V (vs. RHE), the CuCo
alloy exhibited nearly 100% Faraday efficiency (FE) and a high ammonia
production rate of 232.17 mg h-1 mg-1. Stability tests in a simulated
industrial environment showed that the catalyst maintained over 80% FE and an
ammonia production rate exceeding 170 mg h-1 mg-1 over a testing period of 120
hours, outperforming most reported catalysts. To delve deeper into the
synergistic interaction mechanisms between Cu and Co, in situ Raman
spectroscopy was utilized for realtime monitoring, and density functional
theory (DFT) calculations further substantiated our findings. These results not
only highlight the exceptional catalytic performance of the CuCo alloy but also
reflect the effective electronic and energy interactions between the two
metals.