Photoelectrochemical (PEC) solar-fuel conversion is a promising approach to converting energy from sunlight into storable chemical fuels. The development of low cost, highly efficient, and stable semiconductor-based photoelectrodes is a key step in realizing economically viable PEC energy conversion on a global scale. The p-type Cu-based metal oxides possess a wide range of bandgap values and favorable band edges relative to the water splitting redox couples, thus providing promising candidates for PEC solar conversion applications. However, the improvement of the PEC performance for the binary and ternary copper-based metal oxides is severely hindered by the chemical instability and/or unsatisfactory optoelectronic properties. Thus, a fundamental understanding of the key limitations, improvement strategies, and progress of these materials is critical to design high performance and stable photocathodes. Here, we outline the development of p-type binary and ternary Cu-based metal oxide photocathodes, discuss the merits and major challenges of these p-type materials, and present the latest research effort in modifying the materials towards high-performance photocathodes. The critical strategies that have been successfully employed for Cu2O-based solar cells and photocathodes are emphasized to offer guidelines to advance emerging Cu-based photocathodes. Emphasis is placed on the determination of the faradaic efficiency and onset potential of hydrogen generation for the modified photocathodes to properly evaluate the performance and design tandem devices that achieve bias-free solar water splitting. Furthermore, perspectives regarding emerging issues yet to be addressed for the development of Cu-based metal oxide photocathodes with high photocurrent and photovoltage are also presented.

Earth-abundant Cu-based metal oxide photocathodes for photoelectrochemical water splitting

Interfacial engineering is an effective strategy for the design of active oxygen evolution electrode. Yet the intrinsic mechanism of heterogeneous interfaces remains largely unclear for the lack of direct evidence of real active phases. Herein, operando ultraviolet-visible (UV–vis) and Raman spectroscopies were used to probe the surface reconstruction behaviors of [email protected] layered double hydroxides (LDH) hybrid catalysts, which revealed that [email protected] LDH was converted into highly active [email protected] β-Ni(Fe)OOH phases during the OER process. The FeOOH-NiFe LDH interface can promote interfacial charge transfer, delay the Ni oxidation and induce the NiFe LDH phases to highly reactive β-Ni(Fe)OOH. The [email protected] β-Ni(Fe)OOH exhibited excellent OER performance (252 mV at 100 mA cm−2) and a 1.6 times increase (at overpotential of 300 mV) in turnover frequency (TOF) with respect to the active phase γ-Ni(Fe)OOH of NiFe LDH. This work clarifies that ration interface engineering can regulate the generation of highly active phases in the OER process. 

Operando Spectroscopies Unveil Interfacial FeOOH Induced Highly Reactive β-Ni(Fe)OOH for Efficient Oxygen Evolution

Surface chemistry is a pivotal prerequisite besides catalyst composition toward advanced water electrolysis Here, an evident enhancement of the oxygen evolution reaction (OER) is demonstrated on a vanadate-modified iron-nickel catalyst synthesized by a successive ionic layer adsorption and reaction method, which demonstrates ultralow overpotentials of 274 and 310 mV for delivering large current densities of 100 and 400 mA cm-2 , respectively, in 1 m KOH, where vigorous gas bubble evolution occurs Vanadate modification augments the OER activity by i) increasing the electrochemical surface area and intrinsic activity of the active sites, ii) having an electronic interplay with Fe and Ni catalytic centers, and iii) inducing a high surface wettability and a low-gas bubble-adhesion for accelerated mass transport and gas bubble dissipation at large current densities Ex situ and operando Raman study reveals the structural evolution of β-NiOOH and γ-FeOOH phases during the OER through vanadate-active site synergistic interactions Operando dynamic specific resistance measurement evidences an accelerated gas bubble dissipation by a significant decrease in the variation of the interfacial resistance during the OER for the vanadate-modified surface Achievement of a high catalytic turnover of 012 s-1 suggests metallic oxo-anion modification as a versatile catalyst design strategy for advanced water oxidation

Efficient Oxygen Evolution and Gas Bubble Release Achieved by a Low Gas Bubble Adhesive Iron–Nickel Vanadate Electrocatalyst

Facile deposition of porous fluorine doped tin oxide by Dr. Blade method for capacitive applications

In-depth understanding of alkaline hydrogen evolution reaction (HER) not only guides the design of catalysts, but also builds up strong foundation for CO2/N2 reduction reactions that both involves water molecules. In this review, we focused on electrical double layer (EDL) of the cathode where the electrochemical reaction takes place, and analyzed the role of main species in this region, i.e. water molecules, adsorbed H, adsorbed OH/OH− and hydrogen gas bubbles. Through investigating these species inside EDL, the key problems are comprehensively covered, including Janus effect of interfacial water, whether or not Had is unique descriptor for alkaline HER, the influence of OHad on alkaline HER from the viewpoint of thermodynamics and kinetics, the effect of cations in electrolyte, as well as the importance of mass transfer at high current densities. Interactions between the interfacial species, as well as the dynamical changes of EDL during the electrocatalytic reaction are also summarized here. Lastly, an account of the methods for probing molecules/ions inside EDL to reveal the underlying mechanism of alkaline HER was presented.

Inside solid-liquid interfaces: Understanding the influence of the electrical double layer on alkaline hydrogen evolution reaction

The synthesis and characterization of highly stable and conductive F:SnO2 (FTO) nanopyramid arrays are investigated, and their use as scaffolds for water splitting is demonstrated. Current densitie...

Template-Free Nanostructured Fluorine-Doped Tin Oxide Scaffolds for Photoelectrochemical Water Splitting.

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Template-Free Nanostructured Fluorine-Doped Tin Oxide Scaffolds for Photoelectrochemical Water Splitting.