Abstract
The electrochemical nitrogen reduction reaction (NRR) technique has great potential for alleviating the high fossil fuel consumption and carbon emissions of the industrial Haber-Bosch method for ammonia (NH3) synthesis. Moreover, the NRR provides great prospects for fully exploiting renewable energy since NH3 is a promising energy carrier without carbon emissions. However, the development of the NRR technique is limited by the lack of efficient catalysts. Great efforts have been made to develop high-efficiency catalysts thus far, in which density functional theory (DFT) calculations have played an important role in assisting catalyst design. Herein, we summarize the recent catalyst design strategies to boost the NRR performance, i.e., the activity and selectivity. Additionally, representative computational studies are reviewed, accompanied by insights into further improving the catalytic behavior. Finally, we briefly discuss the challenges and opportunities in catalyst design via DFT calculations. The purpose of this review is to motivate more intelligent design strategies for high-efficiency NRR.
摘要
发展电化学氮气还原反应(NRR)的合成氨技术可以有效缓解工 业上的哈伯-博什法合成氨的化石燃料消耗与碳排放问题. 同时, 氨是 一种无碳的能源载体, NRR可以实现可再生能源的转换, 因此具有广阔 的发展前景. 然而, 高效催化剂的缺乏限制了NRR技术的发展. 为此, 人 们对开发高效催化剂进行了广泛的探索, 其中密度泛函理论(DFT)计算 在辅助催化剂设计方面发挥了重要作用. 在本综述中, 我们总结了最近 的催化剂设计策略, 这些策略的目的是提高NRR的催化活性和选择性. 此外, 本综述还回顾了具有代表性的计算工作, 并对进一步改善催化性 能提出了见解. 最后, 本综述简要讨论了通过DFT计算进行催化剂设计 所面临的挑战和机遇. 目的在于指导人们采用更有效的设计策略来实 现高效的NRR过程.
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This work was supported by the National Natural Science Foundation of China (21673095).
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Author contributions Jiang Q supervised the project and conceived the idea. Dai TY wrote the draft. Yang CC revised the manuscript and provided constructive suggestions. All authors discussed and commented on the manuscript.
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Tian-Yi Dai received his BE and PhD degrees from Jilin University in 2018 and 2023, respectively. He is currently working as a postdoctoral fellow at the School of Materials Science and Engineering, Jilin University. His current research focuses on the catalyst design through density functional theory calculations. Some of his studies are carried out in close collaboration with experiments.
Chun-Cheng Yang received his BSc and PhD degrees from Jilin University in 2001 and 2006, respectively. He is currently working as a professor at the School of Materials Science and Engineering, Jilin University. He had worked as a postdoctoral fellow at The University of New South Wales and The University of Sydney for 7 years. His research interests focus on micro- and nano-scale energy materials.
Qing Jiang obtained his PhD degree in chemistry from the University of Stuttgart, Germany in 1990. Since 1992, he has been a professor at the School of Materials Science and Engineering, Jilin University, China. His research interests focus on the synthesis of nanomaterials as well as their applications in catalysis, energy storage and conversion, and interface thermodynamics and kinetics of nanomaterials.
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Dai, TY., Yang, CC. & Jiang, Q. Recent progress on catalyst design of nitrogen reduction reaction by density functional theory. Sci. China Mater. 67, 1101–1123 (2024). https://doi.org/10.1007/s40843-023-2847-1
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DOI: https://doi.org/10.1007/s40843-023-2847-1