Enhanced NH(3) Synthesis from Air in a Plasma Tandem-Electrocatalysis System Using Plasma-Engraved N-Doped Defective MoS(2).
Enhanced NH(3) Synthesis from Air in a Plasma Tandem-Electrocatalysis System Using Plasma-Engraved N-Doped Defective MoS(2).
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DOI：
10.1021/jacsau.3c00087
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发表时间：
2023-05-22
期刊：
影响因子：
8
通讯作者：
Li, Xiaodong
中科院分区：
文献类型：
--
作者：
Zheng, Jiageng;Zhang, Hao;Lv, Jiabao;Zhang, Meng;Wan, Jieying;Gerrits, Nick;Wu, Angjian;Lan, Bingru;Wang, Weitao;Wang, Shuangyin;Tu, Xin;Bogaerts, Annemie;Li, Xiaodong
我们开发了一种可持续的方法，使用等离子体串联电催化系统，通过N2-NOx-NH3途径直接从空气中产生NH3。为了有效地将NO2 -还原为NH3，我们提出了一种由垂直石墨烯阵列（N-MoS2/VGs）上的缺陷n掺杂硫化钼纳米片组成的新型电催化剂。我们使用等离子雕刻工艺在电催化剂中同时形成金属1T相、N掺杂和S空位。该体系在−0.53 V vs RHE条件下NH3的产率为7.3 mg h-1 cm-2，比目前最先进的电化学氮还原反应高出近100倍，是其他混合体系的两倍多。此外，本研究仅实现了2.4 MJ molNH3-1的低能耗。密度泛函理论计算表明，S空位和掺杂N原子在NO2 -选择性还原为NH3的过程中起主导作用。这项研究为利用级联系统高效生产NH3开辟了新的途径。
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.