Zhang Guike, Li Xiaotian, Chen Kai, Guo Yali, Ma Dongwei, Chu Ke
School of Materials Science and Engineering, Lanzhou Jiaotong University, Lanzhou, 730070, China.
Key Laboratory for Special Functional Materials of Ministry of Education, School of Materials Science and Engineering, Henan University, Kaifeng, 475004, China.
Angew Chem Int Ed Engl. 2023 Mar 20;62(13):e202300054. doi: 10.1002/anie.202300054. Epub 2023 Feb 15.
We demonstrate the great feasibility of MBenes as a new class of tandem catalysts for electrocatalytic nitrate reduction to ammonia (NO RR). As a proof of concept, FeB is first employed as a model MBene catalyst for the NO RR, showing a maximum NH -Faradaic efficiency of 96.8 % with a corresponding NH yield of 25.5 mg h cm at -0.6 V vs. RHE. Mechanistic studies reveal that the exceptional NO RR activity of FeB arises from the tandem catalysis mechanism, that is, B sites activate NO to form intermediates, while Fe sites dissociate H O and increase *H supply on B sites to promote the intermediate hydrogenation and enhance the NO -to-NH conversion.
我们证明了MBenes作为一类新型串联催化剂用于电催化硝酸盐还原制氨（NO RR）具有很大的可行性。作为概念验证，首先将FeB用作NO RR的模型MBene催化剂，在相对于可逆氢电极（RHE）为-0.6 V时，显示出最大NH₃法拉第效率为96.8%，相应的NH₃产率为25.5 mg h⁻¹ cm⁻²。机理研究表明，FeB出色的NO RR活性源于串联催化机制，即B位点活化NO形成中间体，而Fe位点使H₂O解离并增加B位点上*H的供应，以促进中间体氢化并增强NO到NH₃的转化。
