Novel Carbon-based Catalyst Developed for Efficient Photo-driven CO2Cycloaddition

Prof. CHEN Liang’s group and Prof. LU Zhiyi’s group at the Ningbo Institute of Materials Technology and Engineering (NIMTE) of Chinese Academy of Sciences (CAS) proposed a highlyactive carbon-based catalyst, which can directly utilize renewable energy (e.g., solar energy) to improve the efficiency of photo-driven CO2cycloaddition effectively. The study was published in Advanced Materials.

The increasing greenhouse gas (mainly CO2) emissions have exacerbated global warming and ocean acidification. To achieve peak CO2emissions before 2030 and carbon neutrality by 2060, the elimination of CO2based on the capture and conversion of CO2is urgently required. Among many strategies to do so, the cycloaddition of CO2with epoxides to generate cyclic carbonates has attracted extensive attention thanks to the diverse application of products.

By a versatile molecule-confined pyrolysis strategy, researchers at NIMTE proposed and synthesized a semiconductive Al-N-C catalyst possessing high density of atomically dispersed Al-N4motifs.

The Al and N species serve as Lewis acid and base sites, respectively, which are combined to facilitate the substrate activation for the photo-driven CO2cycloaddition reactions.

Under light irradiation, the synthesized Al-N-C catalyst showed excellent catalytic performance (≈95% conversion, reaction rate = 3.52 mmol g-1h-1) for the CO2cycloaddition reaction.

In addition, both experimental and theoretical analyses revealed that light irradiation facilitates the photo-generated electron transfer from the semiconductive Al-N-C catalyst to the epoxide reactant, contributing to the high-efficiency formation of a ringopened intermediate through the rate-limiting step. It, therefore, constitutes a new activation mechanism for CO2cycloaddition reaction.

Hence, this study has provided a novel approach for high-efficiency CO2cycloaddition by integrating atomically dispersed Al species and photothermal effect, and may inspire advanced catalyst design.

Contact

YANG Qihao

Ningbo Institute of Materials Technology and Engineering

E-mail: yangqihao@nimte.ac.cn

(NIMTE)