Solid surface frustrated Lewis pair constructed on layered AlOOH for hydrogenation reaction

Shulin Liu; Minghua Dong; Yuxuan Wu; Sen Luan; Yu Xin; Juan Du; Shaopeng Li; Huizhen Liu; Buxing Han

doi:10.1038/s41467-022-29970-6

Solid surface frustrated Lewis pair constructed on layered AlOOH for hydrogenation reaction

Nat Commun. 2022 Apr 28;13(1):2320. doi: 10.1038/s41467-022-29970-6.

Authors

Shulin Liu^#^{1

2}, Minghua Dong^#^{1

2}, Yuxuan Wu^{1

2}, Sen Luan^{1

2}, Yu Xin^{1

2}, Juan Du^{1

2}, Shaopeng Li^{1

2}, Huizhen Liu^{3

4}, Buxing Han^{1

2}

Affiliations

¹ Beijing National Laboratory for Molecular Sciences, CAS Key Laboratory of Colloid and Interface and Thermodynamics, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190, China.
² School of Chemistry and Chemical Engineering, University of Chinese Academy of Sciences, Beijing, 100049, China.
³ Beijing National Laboratory for Molecular Sciences, CAS Key Laboratory of Colloid and Interface and Thermodynamics, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190, China. liuhz@iccas.ac.cn.
⁴ School of Chemistry and Chemical Engineering, University of Chinese Academy of Sciences, Beijing, 100049, China. liuhz@iccas.ac.cn.

^# Contributed equally.

Abstract

Designing heterogeneous solid surface frustrated Lewis pair (ssFLP) catalyst for hydrogenation is a new challenge in catalysis and no research has been reported on the construction of ssFLP on boehmite (AlOOH) surfaces up to now as far as we know. Herein, AlOOH with a layer structure is prepared and it is found that the Lewis basic O_Hv site (one H removed from OH) and an adjacent Lewis acidic unsaturated Al site (Al³⁺_unsatur.) proximal to a surface OH_v (OH vacancy) on AlOOH layers could form the ssFLP. The layered structure of AlOOH and its abundant OH defects over the surface result in a high concentration of O_Hv/Al³⁺_unsatur. FLPs, which are conducive to highly efficient hydrogen activation for hydrogenation of olefins and alkynes with low H-H bond dissociates activation energy of 0.16 eV under mild conditions (T = 80°C and P(H₂) = 2.0 MPa). This work develops a new kind of hydrogenation catalyst and provides a new perspective for creating solid surface FLP.

Abstract

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