Engineering Layered Double Hydroxide–Based Photocatalysts Toward Artificial Photosynthesis: State‐of‐the‐Art Progress and Prospects

Abstract

Layered double hydroxide (LDH) is a class of 2D nanomaterials, which endows auspicious properties for ameliorating the photocatalytic performance in the realm of solar‐to‐chemical production stemming from the chemical versatility of their host layers. However, pristine LDH suffers from slow charge‐carrier mobility, high rate of electron–hole recombination as well as a tendency to agglomerate, rendering them unbefitting for practical use. Due to the aforementioned bottlenecks, structural modifications such as thickness tuning, cocatalyst incorporation, semiconductor coupling, and ternary heterostructure engineering have been extensively investigated to elucidate a new lease of landscape to the burgeoning potential of LDHs toward artificial photosynthesis. This review summarizes a panorama of state‐of‐the‐art advancements related to the synthesis and modification of LDH‐based nanocomposites for enhanced physicochemical properties toward boosted photocatalysis. Particularly, their progress in versatile energy applications in photocatalytic water splitting (hydrogen and oxygen evolution), and nitrogen and carbon dioxide reduction reactions will be systematically presented. Insights into band structures, electronic properties, and charge‐carrier dynamics of LDH‐based nanostructures will be discussed to unravel the structure–performance relationship. Finally, this review will prospect the invigorating prospectives and opportunities in engineering next‐generation LDH‐based photocatalysts with augmented performances to pave new inroads at the forefront of this research.

A current overview of the oxidative desulfurization of fuels utilizing heat and solar light: from materials design to catalysis for clean energy

“…Over the past few years, layered double hydroxide (LDH) has gained copious attention in the field of photocatalysis for its unique 2D-layered structure, remarkable light-capturing ability and tailorable band gap. 248 Huang et al hybridized ZnAl-and ZnCr-LDH with g-C 3 N 4 nanosheets through an electrostatic selfassembly approach to establish a Z-scheme heterojunction to improve the efficiency in light-driven ODS. 249 The Z-scheme heterojunction recombined excited electrons from LDH and holes from g-C 3 N 4 , preserving the free reactive electrons and holes in the CB of g-C 3 N 4 and the VB of LDH, respectively, for redox reactions, which was greatly conducive to the ODS reaction rate (Fig.…”

Progress and Perspectives in Photo‐ and Electrochemical‐Oxidation of Biomass for Sustainable Chemicals and Hydrogen Production

“…[125] Fernández et al employed in situ FTIR and isotopically labeled glycerol ( 13 CH 2 OH 12 CHOH 13 CH 2 OH) to investigate the CC bond cleavage and CO 2 formation on Pt in acidic media. [120,126,127] They have found out that the terminal 13 CH 2 OH groups are easier to electro-oxidize and can happen at low potentials around 0.3 V RHE , while the mass production of 12 CO 2 from the central 12 CHOH group can only be observed above 1.2 V RHE . Li and Harrington covered in detail glycerol electro-oxidation mechanism through an overview of previous studies.…”

“…Nevertheless, up to now most of the reported semiconductors proven to produce H 2 upon water splitting do not display a positive enough valence band for carrying out the sluggish water oxidation. [10][11][12][13][14] Value-added oxidation reactions are a particularly attractive pathway forward to further reduce costs through a reduced energy consumption and added market value. As illustrated in Figure 1, biomass electrolysis as a viable alternative, substitutes the sluggish water oxidation with the thermodynamically more favorable organic molecule oxidation.…”

Fabrication of g-C3N4 Nanosheets Anchored With Controllable CdS Nanoparticles for Enhanced Visible-Light Photocatalytic Performance

“…Semiconductor materials have received widespread attention as promising photocatalysts for clean energy production and environmental problems. ( Tong et al, 2012 ; Chang et al, 2016 ; Yu et al, 2017 ; Qi et al, 2018 ; Cao et al, 2019 ; Ng et al, 2021 ). Recently, g-C 3 N 4 has received considerable attention as a promising photocatalyst, owing to its ease of preparation, high stability, low cost, clean and low toxicity, narrowed bandgap (∼2.7 eV), and special two-dimensional (2D) layered structure ( Shi et al, 2016 ; Teng et al, 2017 ; Han et al, 2018 ; Deng et al, 2019 ; Ong et al, 2020 ; Vu et al, 2020 ; Yu et al, 2021 ); however, diverse drawbacks include poor efficiency of light utilization and low separation of photogenerated charges during the application, making g-C 3 N 4 less attractive for photocatalyst construction.…”