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Crystal defect engineering of Bi2Te3 nanosheets by Ce doping for efficient electrocatalytic nitrogen reduction
Nano Research ( IF 9.5 ) Pub Date : 2023-02-15 , DOI: 10.1007/s12274-022-5319-x
Jianli Nan , Yongqin Liu , Daiyong Chao , Youxing Fang , Shaojun Dong

Electrochemical nitrogen reduction reaction (NRR) is a promising method for the synthesis of ammonia (NH3). However, the electrochemical NRR process remains a great challenge in achieving a high NH3 yield rate and a high Faradaic efficiency (FE) due to the extremely strong N≡N bonds and the competing hydrogen evolution reaction (HER). Recently, bismuth telluride (Bi2Te3) with two-dimensional layered structure has been reported as a promising catalyst for N2 fixation. Herein, to further enhance its NRR activity, a general doping strategy is developed to introduce and modulate the crystal defects of Bi2Te3 nanosheets by adjusting the amount of Ce dopant (denoted as Cex−Bi2Te3, where x represents the designed molar ratio of Ce/Bi). Meanwhile, the crystal defects can be designed and controlled by means of ion substitution and charge compensation. At −0.60 V versus the reversible hydrogen electrode (RHE), Ce0.3−Bi2Te3 exhibits a high NH3 yield (78.2 µg·h−1·mg −1cat ), a high FE (19.3%), and excellent structural and electrochemical stability. Its outstanding catalytic activity is attributed to the tunable crystal defects by Ce doping. This work not only contributes to enhancing the NRR activity of Bi2Te3 nanosheets, but also provides a reliable approach to prepare high-performance electrocatalysts by controlling the type and concentration of crystal defects for artificial N2 fixation.



中文翻译:

掺杂 Ce 的 Bi2Te3 纳米片晶体缺陷工程用于高效电催化氮还原

电化学氮还原反应 (NRR) 是合成氨 (NH 3 ) 的一种很有前途的方法。然而,由于极强的N≡N键和竞争性析氢反应(HER),电化学NRR过程在实现高NH 3产率和高法拉第效率(FE)方面仍然是一个巨大的挑战。最近,据报道具有二维层状结构的碲化铋 (Bi 2 Te 3 ) 是一种很有前途的 N 2固定催化剂。在此,为了进一步增强其 NRR 活性,开发了一种通用掺杂策略来引入和调制 Bi 2 Te 3的晶体缺陷通过调整Ce掺杂量(表示为Ce x -Bi 2 Te 3,其中x代表Ce/Bi的设计摩尔比)来制备纳米片。同时,可以通过离子置换和电荷补偿来设计和控制晶体缺陷。在相对于可逆氢电极 (RHE) -0.60 V 时,Ce 0.3 -Bi 2 Te 3表现出高 NH 3产率(78.2 µg·h -1 ·mg -1 cat ),高 FE (19.3%),以及出色的结构和电化学稳定性。其出色的催化活性归因于 Ce 掺杂的可调晶体缺陷。该工作不仅有助于提高Bi 2 Te 3纳米片的NRR活性,还为通过控制人工N 2固定晶体缺陷的类型和浓度来制备高性能电催化剂提供了可靠的途径。

更新日期:2023-02-15
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