Modelling heterogeneous interfaces for solar water splitting

Abstract

The generation of hydrogen from water and sunlight offers a promising approach for producing scalable and sustainable carbon-free energy. The key of a successful solar-to-fuel technology is the design of efficient, long-lasting and low-cost photoelectrochemical cells, which are responsible for absorbing sunlight and driving water splitting reactions. To this end, a detailed understanding and control of heterogeneous interfaces between photoabsorbers, electrolytes and catalysts present in photoelectrochemical cells is essential. Here we review recent progress and open challenges in predicting physicochemical properties of heterogeneous interfaces for solar water splitting applications using first-principles-based approaches, and highlights the key role of these calculations in interpreting increasingly complex experiments.

Koopmans-Compliant Spectral Functionals for Extended Systems

“…Accurate first-principles predictions of spectral properties-such as band gaps or photoemission spectraattract considerable attention because of their critical role in the design and characterization of optical and electronic devices, e.g., for solar energy harvesting and conversion [1]. To date, the most common approaches to compute these quantities in extended systems are based on many-body perturbation theory (MBPT) using Green's-function-based approaches [2] (such as the GW approximation [3]) or wavefunction-based methods like coupled cluster [4] or quantum Monte Carlo [5], with GW being considered for the case of solids a good compromise between accuracy and computational costs.…”

Determination of the Intrinsic Defect at the Origin of Poor H2 Evolution Performance of the Monoclinic BiVO4 Photocatalyst Using Density Functional Theory

“…[1][2][3] It is an alternative photocatalyst to TiO 2 for organic pollutant removal in gasoline or water via photocatalytic oxidation, e.g thiophene oxidation with loaded Pt and RuO 2 cocatalysts. 4 BiVO 4 is also a common photoanode for photoelectrochemical water splitting for several reasons.…”

“…AgNO 3 ) to improve its activity are utilized, or a small amount of external bias applied, or a hydrogen-producing photocathode is used in a tandem water splitting arrangement. 7,8 Also, BiVO 4 photoanodes do not require the use of strongly acidic or basic media to achieve an optimum photoelectrochemical performance.…”

Mixed‐Metal Tungsten Oxide Photoanode Materials Made by Pulsed‐Laser in Liquids Synthesis

“…The performance of photoelectrodes is not just governed by sunlight absorption, but band edge positions of the material in contact with the liquid electrolyte, material conductivity, carrier lifetimes, and charge recombination processes also matter; structure size critically affects the probability of a photogenerated carrier to reach the photoelectrode-electrolyte interface. [9,16] Since photocurrent generation of complex semiconductors depends on many factors, [46] simple correlations are rarely found, especially when comparing different materials as in this work. Table 1 for nomenclature.…”

“…Detailed understanding of solvation, especially for hydrophilic surfaces with surface defects such as O vacancies at WO3 surfaces, is of key importance. [16] Gerosa et al used firstprinciples calculations to shed light on how structurally inequivalent oxygen vacancies affected charge recombination and optical properties in oxygen-deficient tungsten oxide. [17] We prepared mixed-metal tungsten oxide photoanode nanomaterials by pulsed-laser in liquids synthesis to investigate the effect of ad-metals on optical and photocurrent generation properties.…”