Robust selenium-doped carbon nitride nanotubes for selective electrocatalytic oxidation of furan compounds to maleic acid

Xin Huang; Jinliang Song; Manli Hua; Bingfeng Chen; Zhenbing Xie; Huizhen Liu; Zhanrong Zhang; Qinglei Meng; Buxing Han

doi:10.1039/d1sc01231b

Robust selenium-doped carbon nitride nanotubes for selective electrocatalytic oxidation of furan compounds to maleic acid

Chem Sci. 2021 Apr 1;12(18):6342-6349. doi: 10.1039/d1sc01231b.

Authors

Xin Huang^{1

2}, Jinliang Song^{1

3}, Manli Hua^{1

2}, Bingfeng Chen¹, Zhenbing Xie^{1

2}, Huizhen Liu^{1

2

3}, Zhanrong Zhang¹, Qinglei Meng^{1

3}, Buxing Han^{1

2

3}

Affiliations

¹ Beijing National Laboratory for Molecular Science, CAS Key Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Center for Excellence in Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences Beijing 100190 China songjl@iccas.ac.cn hanbx@icas.ac.cn.
² School of Chemistry and Chemical Engineering, University of Chinese Academy of Sciences Beijing 100049 China.
³ Physical Science Laboratory, Huairou National Comprehensive Science Center Beijing 101400 China.

Abstract

Selective oxidation of biomass-derived furan compounds to maleic acid (MA), an important bulk chemical, is a very attractive strategy for biomass transformation. However, achieving a high MA selectivity remains a great challenge. Herein, we for the first time successfully designed and fabricated Se-doped graphitic carbon nitride nanotubes with a chemical formula of C_3.0N-Se_0.03. The prepared C_3.0N-Se_0.03 was highly efficient for electrocatalytic oxidation of various biomass-derived furan compounds to generate MA. At ambient conditions, the MA yield could reach 84.2% from the electro-oxidation of furfural. Notably, the substituents on the furan ring significantly affected the selectivity to MA, following the order: carboxyl group > aldehyde group > hydroxyl group. Detailed investigation revealed that Se doping could tune the chemical structure of the materials (e.g., C_3.0N-Se_0.03 and g-C₃N₄), thus resulting in the change in catalytic mechanism. The excellent performance of C_3.0N-Se_0.03 originated from the suitable amount of graphitic N and its better electrochemical properties, which significantly boosted the oxidation pathway to MA. This work provides a robust and selective metal-free electrocatalyst for the sustainable synthesis of MA from oxidation of biomass-derived furan compounds.