Сибирский федеральный университет

Тип публикации: статья из журнала

Год издания: 2020

Идентификатор DOI: 10.1021/acsami.0c11487

Ключевые слова: electrochemical nitrogen reduction reaction, ammonia synthesis, nitrogen fixation, au nanoparticles, boron clusters

Аннотация: Currently, the development of stable electrochemical nitrogen reduction reaction (ENRR) catalysts with high N-2 conversion activity and low cost to instead of the traditional Haber-Bosch ammonia production process of high-energy consumption remains a great challenge for researchers. Here, we have immobilized reductive closo-[B12H11](-) boron clusters on a carbon nanotubes (CNT) surface and have successfully prepared a novel Au-CNT catalyst with extraordinary ENRR activity after adding HAuCl4 to the CNT-[B12H11](-) precursor. The excellent properties of ammonia yield (57.7 mu g h(-1) cm(-2)) and Faradaic efficiency (11.97%) make it possible to achieve using this Au-CNT catalyst in large-scale industrial production of ammonia. Furthermore, its outstanding cyclic stability and long-term tolerability performance make it one of the most cost-effective catalysts to date. Here, by means of density functional theory we disclose the associative mechanism of N-2-to-NH3 conversion on the Au(111) surface, providing visual theoretical support for the experimental results.

Журнал: ACS APPLIED MATERIALS & INTERFACES

Выпуск журнала: Vol. 12, Is. 38

Номера страниц: 42821-42831

ISSN журнала: 19448244

Место издания: WASHINGTON

Издатель: AMER CHEMICAL SOC

• Zhao Xue (Wuhan Univ, Coll Chem & Mol Sci, Wuhan 430072, Peoples R China)
• Yang Ziqiong (Wuhan Univ, Coll Chem & Mol Sci, Wuhan 430072, Peoples R China)
• Kuklin Artem (KTH Royal Inst Technol, Sch Engn Sci Chem Biotechnol & Hlth, Div Theoret Chem & Biol, S-10691 Stockholm, Sweden; Siberian Fed Univ, Div Sci & Innovat, Krasnoyarsk 660041, Russia)
• Baryshnikov Glib (KTH Royal Inst Technol, Sch Engn Sci Chem Biotechnol & Hlth, Div Theoret Chem & Biol, S-10691 Stockholm, Sweden; Bohdan Khmelnytsky Natl Univ, Dept Chem & Nanomat Sci, UA-18031 Cherkassy, Ukraine)
• Agren Hans (KTH Royal Inst Technol, Sch Engn Sci Chem Biotechnol & Hlth, Div Theoret Chem & Biol, S-10691 Stockholm, Sweden; Henan Univ, Coll Chem & Chem Engn, Kaifeng 475004, Henan, Peoples R China)
• Zhou Xiaohai (Wuhan Univ, Coll Chem & Mol Sci, Wuhan 430072, Peoples R China; Minist Educ, Engn Res Ctr Organosilicon Cpds & Mat, Wuhan 430072, Peoples R China)
• Zhang Haibo (Wuhan Univ, Coll Chem & Mol Sci, Wuhan 430072, Peoples R China; Wuhan Univ, Natl Demonstrat Ctr Expt Chem, Wuhan 430072, Peoples R China)

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