Liu Honghong, Hai Guangtong, Ding Liang-Xin, Wang Haihui
Guangdong Provincial Key Laboratory of Green Chemical Product Technology, School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou, 510640, China.
Beijing Key Laboratory of Membrane Materials and Engineering, Department of Chemical Engineering, Tsinghua University, Beijing, 100084, China.
Angew Chem Int Ed Engl. 2023 May 2;62(19):e202302124. doi: 10.1002/anie.202302124. Epub 2023 Mar 24.
Electrocatalytic N reduction reaction (NRR) is recognized as a zero-carbon emission method for NH synthesis. However, to date, this technology still suffers from low yield and low selectivity associated with the catalyst. Herein, inspired by the activation of N by lithium metal, a highly reactive defective black phosphorene (D-BP ) is proposed as a lithium-like catalyst for boosting electrochemical N activation. Correspondingly, we also report a strategy for producing environmentally stable D-BP by simultaneously constructing defects and fluorination protection based on topochemical reactions. Reliable performance evaluations show that the fluorine-stabilized D-BP can induce a high NH yield rate of ≈70 μg h mg and a high Faradaic efficiency of ≈26 % at -0.5 V vs. RHE in an aqueous electrolyte. This work not only exemplifies the first stable preparation and practical application of D-BP , but also brings a new design idea for NRR catalysts.
电催化氮还原反应（NRR）被认为是一种用于合成氨的零碳排放方法。然而，迄今为止，该技术仍然存在与催化剂相关的低产率和低选择性问题。在此，受锂金属对氮的活化启发，提出了一种高活性的缺陷黑磷烯（D-BP）作为类锂催化剂来促进电化学氮活化。相应地，我们还报道了一种基于拓扑化学反应同时构建缺陷和氟化保护来制备环境稳定的D-BP的策略。可靠的性能评估表明，在水性电解质中，相对于可逆氢电极（RHE）在-0.5 V时，氟稳定的D-BP可诱导约70 μg h mg的高氨产率和约26%的高法拉第效率。这项工作不仅例证了D-BP的首次稳定制备和实际应用，而且为NRR催化剂带来了新的设计思路。
