Electrochemical CO2 reduction over nitrogen-doped SnO2 crystal surfaces

Abstract

a b s t r a c tCrystal planes of a catalyst play crucial role in determining the electrocatalytic performance for CO 2 reduction. The catalyst SnO 2 can convert CO 2 molecules into valuable formic acid (HCOOH). Incorporating heteroatom N into SnO 2 further improves its catalytic activity. To understand the mechanism and realize a highly efficient CO 2 -to-HCOOH conversion, we used density functional theory (DFT) to calculate the free energy of CO 2 reduction reactions (CO 2 RR) on different crystal planes of N-doped SnO 2 (N-SnO 2 ). The results indicate that N-SnO 2 lowered the activation energy of intermediates leading to a better catalytic performance than pure SnO 2 . We also discovered that the N-SnO 2 (211) plane possesses the most suitable free energy during the reduction process, exhibiting the best catalytic ability for the CO 2 -to-HCOOH conversion. The intermediate of CO 2 RR on N-SnO 2 is HCOO * or COOH * instead of OCHO * . These results may provide useful insights into the mechanism of CO 2 RR, and promote the development of heteroatomdoped catalyst for efficient CO 2 RR.

Ordered cone-structured tin directly grown on carbon paper as efficient electrocatalyst for CO2 electrochemical reduction to formate

“…2 and 4(a-c), it can be observed the OCSn-60 is with the ordered cone-structure, which is composed of four faces with 4 edges. Typical synthesized cone-structure Sn rods have apparent thickness of approximately [5][6][7][8][9][10][11][12][13][14][15][16] lm, and the lengths of the rods are 50-120 lm, which corresponds to a high aspect ratio (length-to-width ratio). Another notable feature in the SEM observations is that the rods are almost perpendicular to the surface of the TCP substrate.…”

“…Different strategies and new designs were explored to improve the performances of Sn-based catalysts [14,15]. The introduction of oxygen, carbon support as well as alloying with other metals was investigated to improve the CO 2 reduction performances, suggesting that such neighboring species can alter the electrical structures of the active Sn sites.…”

Engineering Sn‐based Catalytic Materials for Efficient Electrochemical CO2 Reduction to Formate

“…Among these materials, Sn is an attractive metal for CO 2 reduction due to its relatively low cost compared to noble metals and its environmental friendliness due to its abundance and non‐toxic nature. Sn catalysts have displayed high Faradaic efficiencies and selectivity for CO 2 conversion to formate and exhibit performance tunability through morphology and nanostructure engineering, doping and alloying [40–47] . Product tunability to CO has also been demonstrated with similar strategies mentioned above [48–50] .…”

Nanoporous structured Sn‐MWCNT/Cu electrodes fabricated by electrodeposition–chemical dezincification for catalytic CO2 reduction

“…[22][23][24] In this regard, Sn as a nontoxic and nonprecious metal has attracted much attention with high selectivity, cost effectiveness, environmental friendliness, and stability. 20,25 So far, some impressive results have been achieved with Sn-based catalysts for ERCO 2 , as summarized in Table S1. The morphology of the material has a very important effect on the performance of the catalyst.…”