Enhanced NH3 Synthesis from Air in a Plasma Tandem- Electrocatalysis System Using Plasma-Engraved N-Doped Defective MoS2

被引：21

作者：

Zheng, Jiageng ^{[1
]}

Zhang, Hao ^{[1
]}

Lv, Jiabao ^{[1
]}

Zhang, Meng ^{[2
]}

Wan, Jieying ^{[1
]}

Gerrits, Nick ^{[3
]}

Wu, Angjian ^{[1
]}

Lan, Bingru ^{[1
]}

Wang, Weitao ^{[4
]}

Wang, Shuangyin ^{[5
]}

Tu, Xin ^{[4
]}

Bogaerts, Annemie ^{[3
]}

Li, Xiaodong ^{[1
]}

机构：

[1] Zhejiang Univ, Acad Ecol Civilizat, Coll Energy & Engn, State Key Lab Clean Energy Utilizat, Hangzhou 310027, Peoples R China

[2] Zhejiang Univ, Coll Opt Sci & Engn, Hangzhou 310027, Peoples R China

[3] Univ Antwerp, Dept Chem, Res Grp PLASMANT, B-2610 Antwerp, Belgium

[4] Univ Liverpool, Dept Elect Engn & Elect, Liverpool L69 3GJ, Lancashire, England

[5] Hunan Univ, Coll Chem & Chem Engn, State Key Lab Chem Biosensing & Chemometr, Changsha 410082, Peoples R China

来源：

JACS AU | 2023年 / 3卷 / 05期

基金：

英国工程与自然科学研究理事会; 中国国家自然科学基金;

关键词：

sustainable NH3 production; plasma electrocatalysis; defective N-MoS2; plasma engraving; density functional theory; NITROGEN REDUCTION; AMMONIA; EFFICIENT; MOLYBDENUM; FIXATION; PERFORMANCE; INTERFACE; MECHANISM; LAYER; WATER;

D O I：

10.1021/jacsau.3c00087

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

We have developed a sustainable method to produce NH3 directly from air using a plasma tandem-electrocatalysis system that operates via the N2-NOx-NH3 pathway. To efficiently reduce NO2- to NH3, we propose a novel electrocatalyst consisting of defective N-doped molybdenum sulfide nanosheets on vertical graphene arrays (N-MoS2/VGs). We used a plasma engraving process to form the metallic 1T phase, N doping, and S vacancies in the electrocatalyst simultaneously. Our system exhibited a remarkable NH3 production rate of 7.3 mg h-1 cm-2 at -0.53 V vs RHE, which is almost 100 times higher than the state-of-the-art electrochemical nitrogen reduction reaction and more than double that of other hybrid systems. Moreover, a low energy consumption of only 2.4 MJ molNH3-1 was achieved in this study. Density functional theory calculations revealed that S vacancies and doped N atoms play a dominant role in the selective reduction of NO2- to NH3. This study opens up new avenues for efficient NH3 production using cascade systems.

引用

页码：1328 / 1336

页数：9

共 71 条

[1] Hierarchical hollow nanotubes of NiFeV-layered double hydroxides@CoVP heterostructures towards efficient, pH-universal electrocatalytical nitrogen reduction reaction to ammonia [J].