Constructing Single-atom Ni on N-doped Carbon Via Chelation-anchored Strategy for the Hydrogenolysis of Lignin
Tianjin Li1,4, Bo Chen1, Meifang Cao1, Xinping Ouyang1*, Xueqing Qiu2, Changzhi Li3*
1. School of Chemistry and Chemical Engineering, Guangdong Provincial Key Lab of Green Chemical Product Technology, South China University of Technology, Guangzhou 510640, P. R. China.
2 School of Chemical Engineering and Light Industry, Guangdong University of Technology, Guangzhou 510006, P. R. China.
3CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Dalian 116023, P.R. China.
4Shandong Provincial Key Laboratory of Biomass Gasification Technology, Energy Research Institute, Qilu University of Technology (Shandong Academy of Sciences), Jinan 250014, P.R China.
*Authors to whom any correspondence should be addressed.
E-mail: ceouyang@scut.edu.cn (Xinping Ouyang); licz@dicp.ac.cn (Changzhi Li).
ABSTRACT
The efficient utilization of lignin remains a great challenge due to its complex non-repetitive structure and the lack of efficient catalyst. Herein, a single-atom catalyst Ni@N-C was designed via a facile chelation-anchored strategy. Ni atoms were immobilized on the N-doped carbon carrier by a two-stage pyrolysis of a mixture of D-glucosamine hydrochloride, nickel acetate and melamine. D-glucosamine hydrochloride as a chelating agent prevented the aggregation of Ni2+, and melamine provided enough N to anchor Ni by forming Ni-N4structure. Ni@N-C gave a 31.2% yield of aromatic compounds from lignin hydrogenolysis, which was twice higher than that achieved by Ni cluster catalyst. Based on the experimental and DFT calculation results, the higher activity of Ni@N-C was attributed to its lower H2 dissociation energy and the reduced energy barriers of the transition states. The strategy described opens an efficient green avenue for preparing single-atom catalyst that possesses outstanding activity in lignin depolymerization.