Two-dimensional forms of robust CO2 reduction photocatalysts

Abstract

Photoelectrocatalysts that use sunlight to power the CO 2 reduction reaction will be crucial for carbon-neutral power and energyefficient industrial processes. Scalable photoelectrocatalysts must satisfy a stringent set of criteria, such as stability under operating conditions, product selectivity, and efficient light absorption. Two-dimensional materials can offer high specific surface area, tunability, and potential for heterostructuring, providing a fresh landscape of candidate catalysts. From a set of promising bulk CO 2 reduction photoelectrocatalysts, we screen for candidate monolayers of these materials, then study their catalytic feasibility and suitability. For stable monolayer candidates, we verify the presence of visible-light band gaps, check that band edges can support CO 2 reduction, determine exciton binding energies, and compute surface reactivity. We find visible light absorption for SiAs, ZnTe, and ZnSe monolayers, and that due to a lack of binding, CO selectivity is possible. We thus identify SiAs, ZnTe, and ZnSe monolayers as targets for further investigation, expanding the chemical space for CO 2 photoreduction candidates.

Computational Synthesis of 2D Materials: A High-throughput Approach to Materials Design

“…Both the 1T and 2H phase for NbO 2 possess high ∆E f vac , as shown by the red shaded region in Figure 5, making substrate-assisted synthesis methods the most feasible method to synthesize these 2D films. The ∆E f vac 's in Figure 5 are consistent with prior computational [16,34] and experimental work [40].…”

“…To demonstrate the functionalities of the Hetero2d package, we screened for suitable substrates for four 2D materials, namely 2H-MoS 2 , 1T -NbO 2 , 2H-NbO 2 [16], and hexagonal-ZnTe [34]. The four 2D materials in consideration possess hexagonal symmetry as illustrated in Figure 3.…”

“…MoS 2 was selected because there is a large amount of experimental and computational [35,36,37,20] data available in literature which we can use to validate the computed properties from our Hetero2d workflow. The hexagonal-ZnTe [34], 1T -NbO 2 , and 2H-NbO 2 [16] are yet to be synthesized. In addition, these particular 2D materials have diverse predicted properties see Table 2.…”

“…In addition, these particular 2D materials have diverse predicted properties see Table 2. It is noteworthy that hexagonal-ZnTe has been predicted to be an excellent CO 2 reduction photocatalyst [34]. The properties of a 2D material can differ when placed on different millerindex planes for the same substrate.…”

Data-driven studies of magnetic two-dimensional materials

“… and were also ML recommended structures which we excluded because of the radioactive elements they contain. The recommendations we generated can then be subjected to additional screening with more computationally expensive tests for chemical stability 73 , 74 , such as calculations of the dynamic stability 75 , 76 . The most promising results will serve as viable options for materials synthesis and experimental verification.…”