Highly Selective Photocatalytic CO₂ Methanation with Water Vapor on Single‐Atom Platinum‐Decorated Defective Carbon Nitride

Abstract

Solar‐driven CO2 methanation with water is an important route to simultaneously address carbon neutrality and produce fuels. It is challenging to achieve high selectivity in CO2 methanation due to competing reactions. Nonetheless, aspects of the catalyst design can be controlled with meaningful effects on the catalytic outcomes. We report highly selective CO2 methanation with water vapor using a photocatalyst that integrates polymeric carbon nitride (CN) with single Pt atoms. As revealed by experimental characterization and theoretical simulations, the widely explored Pt−CN catalyst is adapted for selective CO2 methanation with our rationally designed synthetic method. The synthesis creates defects in CN along with formation of hydroxyl groups proximal to the coordinated Pt atoms. The photocatalyst exhibits high activity and carbon selectivity (99 %) for CH4 production in photocatalytic CO2 reduction with pure water. This work provides atomic scale insight into the design of photocatalysts for selective CO2 methanation.

Activated g-C3N4 Photocatalyst with Defect Engineering for Efficient Reduction of CO2 in Water

“…46 As shown in Figure 4c, the PL spectrum of dCN displayed a high intrinsic emission peak due to the existing plentiful carrier recombination centers. 23 Compared to dCN, t-dCN revealed a stronger intrinsic emission peak. However, after the introduction of TiO 2 during boiling water treatment, P25/t-dCN exhibited the relative damped emission, showing the reduced carrier recombination rate.…”

2D/2D g-C 3 N 4 /BiOCl with oxygen vacancy heterostructure by grinding for improved visible-light-driven photocatalyst

“…In Fig. 2b, the main peak of the CN/BOC-5 composite at 288.2 eV can be attributed to the N-C = N bond [29] from CN, while the C peak at 284.7 eV should come from the adsorption of impurity carbon by BOC [30]. It can be seen from Fig.…”

“…It can be seen from Fig. 2c that there are four peaks in the N 1S spectrum of CN at 398.7, 400.1, 401.2, and 404.5 eV, which represent the N in C-N = C, C-N-H, N-(C) 3 , and π-excitation, respectively [30].…”

Recent advances of single-atom catalysts in CO2conversion

“…17i). 316 Considering the merit of dual-metal single atom, Pan er al. fabricated a dual SA of Pt and Cu decorated on self-doped-TiO 2 nanotubes (Pt-Au/R-TNTs).…”