Self-oriented Sb<sub>2</sub>Se<sub>3</sub> nanoneedle photocathodes for water splitting obtained by a simple spin-coating method

Kim, Jimin; Yang, Wooseok; Oh, Yunjung; Lee, Hyungsoo; Lee, Seonhee; Shin, Hyunjung; Kim, Joosun; Moon, Jooho

doi:10.1039/c6ta09602f

Cited by 97 publications

(103 citation statements)

References 41 publications

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“…The H 2 produced from the water was also monitored under similar operation conditions by gas chromatography (GC) as shown in Figure S12 (Supporting Information). [51] By comparing detected hydrogen gas with the expected amount obtained by the photocurrent, the faradaic efficiency (i.e., the ratio of the rate of H 2 evolution to that of e − /2) can be calculated.…”

Section: Resultsmentioning

confidence: 99%

Boosting Visible Light Harvesting in p‐Type Ternary Oxides for Solar‐to‐Hydrogen Conversion Using Inverse Opal Structure

Yang

Tan

et al. 2019

Adv Funct Materials

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P-type semiconductors based on ternary oxides have attracted wide interest owing to their earth-crust abundance and favorable optoelectronic properties. Among the p-type ternary oxides, delafossite-phase CuFeO 2 has received considerable attention because it has the potential to fully harness visible light (<800 nm) owing to its narrow bandgap (1.4-1.6 eV). Despite the favorable optoelectronic properties predicted by theoretical studies, CuFeO 2 photocathodes have low quantum efficiency under visible light near the bandgap edge, which is a major bottleneck for efficient solar-to-hydrogen conversion. Herein, a novel method is presented for boosting visible-light harvesting in the CuFeO 2 photocathode by employing an inverse opal structure as a periodic macrostructure. The periodic macroporous structure allows exceptional near-bandgap photon harvesting, particularly within the range of 600-700 nm, owing to the enhanced light absorption due to multiple scattering together with the short diffusion distance for minority carriers toward the electrolyte. After surface modification with a low-cost double hydroxide electrocatalyst, our CuFeO 2 -based photocathode exhibits a record-breaking photocurrent density of 5.2 mA cm −2 at −0.1 V with respect to the reversible hydrogen electrode for water reduction among p-type ternary oxide-based photocathodes.

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Section: Resultsmentioning

confidence: 99%

Boosting Visible Light Harvesting in p‐Type Ternary Oxides for Solar‐to‐Hydrogen Conversion Using Inverse Opal Structure

Yang

Tan

et al. 2019

Adv Funct Materials

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“…It has also been reported that Sb 2 Se 3 is intrinsically stable towards photocorrosion in strong acidic media unlike Cu 2 O, which is vulnerable to photocorroson 22 . Owing to these merits, the photocurrent density of the Sb 2 Se 3 photocathode has improved rapidly from the initially reported value of 2.5 mA cm −2 to 17.5 cm −2 at 0 V against the reversible hydrogen electrode (RHE) over the short period of its development [23][24][25][26] . However, it is still far below the theoretical maximum (about 40 mA cm −2 , assuming a 1.2 eV E g and a 100% incident photon-to-current efficiency (IPCE)).…”

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Benchmark performance of low-cost Sb2Se3 photocathodes for unassisted solar overall water splitting

et al. 2020

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Determining cost-effective semiconductors exhibiting desirable properties for commercial photoelectrochemical water splitting remains a challenge. Herein, we report a Sb 2 Se 3 semiconductor that satisfies most requirements for an ideal high-performance photoelectrode, including a small band gap and favourable cost, optoelectronic properties, processability, and photocorrosion stability. Strong anisotropy, a major issue for Sb 2 Se 3 , is resolved by suppressing growth kinetics via close space sublimation to obtain high-quality compact thin films with favourable crystallographic orientation. The Sb 2 Se 3 photocathode exhibits a high photocurrent density of almost 30 mA cm −2 at 0 V against the reversible hydrogen electrode, the highest value so far. We demonstrate unassisted solar overall water splitting by combining the optimised Sb 2 Se 3 photocathode with a BiVO 4 photoanode, achieving a solar-tohydrogen efficiency of 1.5% with stability over 10 h under simulated 1 sun conditions employing a broad range of solar fluxes. Low-cost Sb 2 Se 3 can thus be an attractive breakthrough material for commercial solar fuel production.

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“…Cu 2 ZnSn(S,Se) 4 , [14] and Sb 2 Se 3 , [15] for which TiO 2 is mostly produced via atomic layer deposition (ALD), allowing for conformal deposition regardless of the surface morphologies. [18] Although TiO 2 protection improved the stability of photocathodes to some extent compared with their unprotected counterparts, a gradual photocurrent degradation was still unavoidable.…”

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Fullerene as a Photoelectron Transfer Promoter Enabling Stable TiO₂‐Protected Sb₂Se₃ Photocathodes for Photo‐Electrochemical Water Splitting

Tan

Yang

et al. 2019

Advanced Energy Materials

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Understanding the degradation mechanisms of photoelectrodes and improving their stability are essential for fully realizing solar‐to‐hydrogen conversion via photo‐electrochemical (PEC) devices. Although amorphous TiO2 layers have been widely employed as a protective layer on top of p‐type semiconductors to implement durable photocathodes, gradual photocurrent degradation is still unavoidable. This study elucidates the photocurrent degradation mechanisms of TiO2‐protected Sb2Se3 photocathodes and proposes a novel interface‐modification methodology in which fullerene (C60) is introduced as a photoelectron transfer promoter for significantly enhancing long‐term stability. It is demonstrated that the accumulation of photogenerated electrons at the surface of the TiO2 layer induces the reductive dissolution of TiO2, accompanied by photocurrent degradation. In addition, the insertion of the C60 photoelectron transfer promoter at the Pt/TiO2 interface facilitates the rapid transfer of photogenerated electrons out of the TiO2 layer, thereby yielding enhanced stability. The Pt/C60/TiO2/Sb2Se3 device exhibits a high photocurrent density of 17 mA cm−2 and outstanding stability over 10 h of operation, representing the best PEC performance and long‐term stability compared with previously reported Sb2Se3‐based photocathodes. This research not only provides in‐depth understanding of the degradation mechanisms of TiO2‐protected photocathodes, but also suggests a new direction to achieve durable photocathodes for photo‐electrochemical water splitting.

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Self-oriented Sb₂Se₃ nanoneedle photocathodes for water splitting obtained by a simple spin-coating method

Abstract: Sb2Se3 nanoneedles for use as a photocathode for water splitting are fabricated by facile spin-coating. After sequential surface modification with n-TiO2 and Pt, a remarkable photocurrent of 2 mA cm−2 at 0 VRHE is realized.

Cited by 97 publications

References 41 publications

Boosting Visible Light Harvesting in p‐Type Ternary Oxides for Solar‐to‐Hydrogen Conversion Using Inverse Opal Structure

Boosting Visible Light Harvesting in p‐Type Ternary Oxides for Solar‐to‐Hydrogen Conversion Using Inverse Opal Structure

Benchmark performance of low-cost Sb2Se3 photocathodes for unassisted solar overall water splitting

Fullerene as a Photoelectron Transfer Promoter Enabling Stable TiO₂‐Protected Sb₂Se₃ Photocathodes for Photo‐Electrochemical Water Splitting

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Self-oriented Sb2Se3 nanoneedle photocathodes for water splitting obtained by a simple spin-coating method

Abstract: Sb2Se3 nanoneedles for use as a photocathode for water splitting are fabricated by facile spin-coating. After sequential surface modification with n-TiO2 and Pt, a remarkable photocurrent of 2 mA cm−2 at 0 VRHE is realized.

Cited by 97 publications

References 41 publications

Boosting Visible Light Harvesting in p‐Type Ternary Oxides for Solar‐to‐Hydrogen Conversion Using Inverse Opal Structure

Boosting Visible Light Harvesting in p‐Type Ternary Oxides for Solar‐to‐Hydrogen Conversion Using Inverse Opal Structure

Benchmark performance of low-cost Sb2Se3 photocathodes for unassisted solar overall water splitting

Fullerene as a Photoelectron Transfer Promoter Enabling Stable TiO2‐Protected Sb2Se3 Photocathodes for Photo‐Electrochemical Water Splitting

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Self-oriented Sb₂Se₃ nanoneedle photocathodes for water splitting obtained by a simple spin-coating method

Fullerene as a Photoelectron Transfer Promoter Enabling Stable TiO₂‐Protected Sb₂Se₃ Photocathodes for Photo‐Electrochemical Water Splitting