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Theoretical Insights into the Mechanism of Selective Nitrate‐to‐Ammonia Electroreduction on Single‐Atom Catalysts
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2020-12-21 , DOI: 10.1002/adfm.202008533 Huan Niu 1 , Zhaofu Zhang 2 , Xiting Wang 1 , Xuhao Wan 1 , Chen Shao 1 , Yuzheng Guo 1
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2020-12-21 , DOI: 10.1002/adfm.202008533 Huan Niu 1 , Zhaofu Zhang 2 , Xiting Wang 1 , Xuhao Wan 1 , Chen Shao 1 , Yuzheng Guo 1
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Selective nitrate‐to‐ammonia electrochemical conversion is an efficient pathway to solve the pollution of nitrate and an attractive strategy for low‐temperature ammonia synthesis. However, current studies for nitrate electroreduction (NO3RR) mainly focus on metal‐based catalysts, which remains challenging because of the poor understanding of the catalytic mechanism. Herein, taking single transition metal atom supported on graphitic carbon nitrides (g‐CN) as an example, the NO3RR feasibility of single‐atom catalysts (SACs) is first demonstrated by using density functional theory calculations. The results reveal that highly efficient NO3RR toward NH3 can be achieved on Ti/g‐CN and Zr/g‐CN with low limiting potentials of −0.39 and −0.41 V, respectively. Furthermore, the considerable energy barriers are observed during the formation of byproducts NO2, NO, N2O, and N2 on Ti/g‐CN and Zr/g‐CN, guaranteeing their high selectivity. This work provides a new route for the application of SACs and paves the way to the development of NO3RR.
中文翻译：
对单原子催化剂上选择性硝酸盐-氨电还原机理的理论见解
选择性硝酸盐到氨的电化学转化是解决硝酸盐污染的有效途径，并且是低温氨合成的有吸引力的策略。但是，目前对硝酸盐电还原（NO 3 RR）的研究主要集中在金属基催化剂上，由于对催化机理的了解不多，因此仍具有挑战性。在此，以负载在石墨碳氮化物（g-CN）上的单过渡金属原子为例，首先通过密度泛函理论计算证明了单原子催化剂（SAC）的NO 3 RR可行性。结果表明，高效的NO 3 RR对NH 3Ti / g-CN和Zr / g-CN可以分别以-0.39和-0.41 V的低限制电势实现。此外，在Ti / g-CN和Zr / g-CN上形成副产物NO 2，NO，N 2 O和N 2的过程中观察到了相当大的能垒，从而确保了它们的高选择性。这项工作为SAC的应用提供了一条新途径，为NO 3 RR的开发铺平了道路。
更新日期：2020-12-21
中文翻译：
对单原子催化剂上选择性硝酸盐-氨电还原机理的理论见解
选择性硝酸盐到氨的电化学转化是解决硝酸盐污染的有效途径，并且是低温氨合成的有吸引力的策略。但是，目前对硝酸盐电还原（NO 3 RR）的研究主要集中在金属基催化剂上，由于对催化机理的了解不多，因此仍具有挑战性。在此，以负载在石墨碳氮化物（g-CN）上的单过渡金属原子为例，首先通过密度泛函理论计算证明了单原子催化剂（SAC）的NO 3 RR可行性。结果表明，高效的NO 3 RR对NH 3Ti / g-CN和Zr / g-CN可以分别以-0.39和-0.41 V的低限制电势实现。此外，在Ti / g-CN和Zr / g-CN上形成副产物NO 2，NO，N 2 O和N 2的过程中观察到了相当大的能垒，从而确保了它们的高选择性。这项工作为SAC的应用提供了一条新途径，为NO 3 RR的开发铺平了道路。
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