A Transparent, High‐Performance, and Stable Sb₂S₃ Photoanode Enabled by Heterojunction Engineering with Conjugated Polycarbazole Frameworks for Unbiased Photoelectrochemical Overall Water Splitting Devices

Abstract

Developing low‐cost, high‐performance, and durable photoanodes is essential in solar‐driven photoelectrochemical (PEC) energy conversion. Sb2S3 is a low‐bandgap (≈1.7 eV) n‐type semiconductor with a maximum theoretical solar conversion efficiency of ≈28% for PEC water splitting. However, bulk Sb2S3 exhibits opaque characteristics and suffers from severe photocorrosion, and thus the use of Sb2S3 as a photoanode material remains underexploited. This study describes the design and fabrication of a transparent Sb2S3‐based photoanode by conformably depositing a thin layer of conjugated polycarbazole frameworks (CPF‐TCzB) onto the Sb2S3 film. This structural design creates a type‐II heterojunction between the CPF‐TCzB and the Sb2S3 with a suitable band‐edge energy offset, thereby, greatly enhancing the charge separation efficiency. The CPF‐TCzB/Sb2S3 hybrid photoanode exhibits a remarkable photocurrent density of 10.1 mA cm−2 at 1.23 V vs reversible hydrogen electrode. Moreover, the thin CPF‐TCzB overlayer effectively inhibits photocorrosion of the Sb2S3 and enables long‐term operation for at least 100 h with ≈10% loss in photocurrent density. Furthermore, a standalone unbiased PEC tandem device comprising a CPF‐TCzB/Sb2S3 photoanode and a back‐illuminated Si photocathode can achieve a record solar‐to‐hydrogen conversion efficiency of 5.21%, representing the most efficient PEC water splitting device of its kind.

PtTe2/Sb2S3 Nanoscale Heterostructures for the Photocatalytic Direct Z-Scheme with High Solar-to-Hydrogen Efficiency: A Theoretical Investigation

“…This direction of the E built‑in and the band alignments of the two configurations support them to work as a Z-scheme rather than type-II photocatalytic performance. Additionally, the present band alignments and direction of the built-in electric field are similar to those of the p–n heterojunctions containing PtTe 2 or Sb 2 S 3 , ,, implying that a weak p–n heterojunction may also occur in the present heterostructure. As shown in Figure , the E built‑in accelerates the recombination of the photogenerated hole at the VBM of the PtTe 2 monolayer and the electron at the CBM of the Sb 2 S 3 monolayer.…”

“…Sb 2 S 3 as a member of the antimony chalcogenide compounds and an n-type semiconductor has been widely applied in the fields of the photovoltaic device in view of its excellent stability, earth abundance, good light harvesting, and easy to prepare. 24 Li et al 25 synthesized the pristine crystalline Sb 2 S 3 and found that it has a very narrow band gap of about 1.55 eV. Perales et al 26 obtained Sb 2 S 3 multilayers by physical vapor deposition on class substrates and made a comparison of the material properties between multilayer and monolayer.…”

“…Recently, the potential use of the PtTe 2 monolayer in a variety of different applications, such as electrocatalysis, ultrafast photonics, and terahertz photodetection, has been reported. Sb 2 S 3 as a member of the antimony chalcogenide compounds and an n-type semiconductor has been widely applied in the fields of the photovoltaic device in view of its excellent stability, earth abundance, good light harvesting, and easy to prepare . Li et al synthesized the pristine crystalline Sb 2 S 3 and found that it has a very narrow band gap of about 1.55 eV.…”

Nanogels as Novel Nanocarrier Systems for Efficient Delivery of CNS Therapeutics

“…The results reported by Alvarez et al suggest that the induction of a neurodegenerative disease may depend on the size and concentration of the nanoparticles and on their biocompatibility ( Oberdörster, 2010 ). Current data of the assessments of the toxicity of the nanomaterials suggest that rigorous in vitro , in vivo , and clinical toxicity studies are needed before the clinical transformation of the nanomaterials can be achieved ( Wang et al, 2022 ). Emphasis on detailed toxicity studies of nanogels is needed to provide evolutionary insight into the risks associated with efficient applications of these promising targeting approaches.…”

Bifunctional thioacetamide-mediated synthesis of few-layered MoOSx nanosheet-modified CdS hollow spheres for efficient photocatalytic H2 production

“…1–7 Particularly, photocatalytic hydrogen (H 2 ) production, utilizing inexhaustible solar energy as the driving force, is of paramount importance to lessen the global energy shortage and environmental crisis. 8–12 To date, manifold semiconductor materials have been employed as host photocatalysts and widely used for sustainable H 2 production via photocatalytic water splitting. 13–17 Among them, hollow-structured materials are emerging as significant functional photocatalysts to achieve efficient photocatalytic H 2 -generation rate owing to their outstanding merits, such as multiple light reflections, large specific surface area, and shortened charge transport length.…”