{"title":"Dual back interface engineering optimized charge carrier dynamics in Sb2(S,Se)3 photocathodes for efficient solar hydrogen production†","authors":"Hafiz Sartaj Aziz, Tahir Imran, Munir Ahmad, Guo-Jie Chen, Ping Luo, Dong-Lou Ren, Bing-Suo Zou, Ju-Guang Hu, Zheng-Hua Su, Pei-Guang Yan, Guang-Xing Liang and Shuo Chen","doi":"10.1039/D4SC05893C","DOIUrl":null,"url":null,"abstract":"<p >Antimony sulfoselenide (Sb<small><sub>2</sub></small>(S,Se)<small><sub>3</sub></small>) is a promising sunlight absorber material for solar energy conversion in photovoltaic (PV) cells and photoelectrochemical (PEC) photoelectrodes due to its excellent photoelectric properties. However, the obtained thin-film and back contact properties significantly influence the PEC performance of photocathodes, causing severe bulk recombination, carrier transport loss, and deteriorating half-cell solar-to-hydrogen (HC-STH) efficiency. This study introduces an intriguing dual back interface engineering strategy for Sb<small><sub>2</sub></small>(S,Se)<small><sub>3</sub></small> photocathodes by incorporating an intermediate MoO<small><sub>2</sub></small> layer and a secondary carrier transport channel of Au to strengthen charge carrier dynamics. The synergistic assembly of these dual back interface layers improves the growth kinetics and achieves the optimal orientation of Sb<small><sub>2</sub></small>(S,Se)<small><sub>3</sub></small> thin films by increasing substrate wettability. Moreover, by shortening the back contact barrier height and passivating defect-assisted recombinations, these dual back underlayers simultaneously enhance carrier transport and separation efficiencies. As a result, the photocurrent density of the champion Sb<small><sub>2</sub></small>(S,Se)<small><sub>3</sub></small> photocathode increases from 5.89 to 32.60 mA cm<small><sup>−2</sup></small>, and the HC-STH conversion efficiency improves significantly from 0.30% to 3.58%, representing the highest value for Sb<small><sub>2</sub></small>(S,Se)<small><sub>3</sub></small>-based photocathodes. This work highlights the effectiveness of dual back interface engineering in promoting the PEC performance of chalcogenide photocathodes for solar hydrogen evolution applications.</p>","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":" 1","pages":" 393-409"},"PeriodicalIF":7.6000,"publicationDate":"2024-12-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/sc/d4sc05893c?page=search","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chemical Science","FirstCategoryId":"92","ListUrlMain":"https://pubs.rsc.org/en/content/articlelanding/2025/sc/d4sc05893c","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
Abstract
Antimony sulfoselenide (Sb2(S,Se)3) is a promising sunlight absorber material for solar energy conversion in photovoltaic (PV) cells and photoelectrochemical (PEC) photoelectrodes due to its excellent photoelectric properties. However, the obtained thin-film and back contact properties significantly influence the PEC performance of photocathodes, causing severe bulk recombination, carrier transport loss, and deteriorating half-cell solar-to-hydrogen (HC-STH) efficiency. This study introduces an intriguing dual back interface engineering strategy for Sb2(S,Se)3 photocathodes by incorporating an intermediate MoO2 layer and a secondary carrier transport channel of Au to strengthen charge carrier dynamics. The synergistic assembly of these dual back interface layers improves the growth kinetics and achieves the optimal orientation of Sb2(S,Se)3 thin films by increasing substrate wettability. Moreover, by shortening the back contact barrier height and passivating defect-assisted recombinations, these dual back underlayers simultaneously enhance carrier transport and separation efficiencies. As a result, the photocurrent density of the champion Sb2(S,Se)3 photocathode increases from 5.89 to 32.60 mA cm−2, and the HC-STH conversion efficiency improves significantly from 0.30% to 3.58%, representing the highest value for Sb2(S,Se)3-based photocathodes. This work highlights the effectiveness of dual back interface engineering in promoting the PEC performance of chalcogenide photocathodes for solar hydrogen evolution applications.
硫代硒化锑(Sb2(S,Se)3)由于其优异的光电性能,是一种很有前途的太阳能吸收材料,可用于光伏电池和光电化学(PEC)光电电极的太阳能转换。然而,所获得的薄膜和背接触特性显著影响光电阴极的PEC性能,导致严重的体复合、载流子输运损失和半电池太阳能制氢(HC-STH)效率下降。本研究提出了一种有趣的Sb2(S,Se)3光电阴极的双后界面工程策略,通过引入中间MoO2层和Au的二次载流子传输通道来增强载流子动力学。这些双背界面层的协同组装改善了Sb2(S,Se)3薄膜的生长动力学,并通过提高衬底润湿性实现了Sb2(S,Se)3薄膜的最佳取向。此外,通过缩短背接触势垒高度和钝化缺陷辅助重组,这些双背底层同时提高了载流子输运和分离效率。结果表明,冠军Sb2(S,Se)3光电阴极的光电流密度从5.89增加到32.60 mA cm−2,HC-STH转换效率从0.30%显著提高到3.58%,达到了Sb2(S,Se)3基光电阴极的最高值。本工作强调了双后界面工程在提高太阳能析氢硫化物光电阴极PEC性能方面的有效性。
期刊介绍:
Chemical Science is a journal that encompasses various disciplines within the chemical sciences. Its scope includes publishing ground-breaking research with significant implications for its respective field, as well as appealing to a wider audience in related areas. To be considered for publication, articles must showcase innovative and original advances in their field of study and be presented in a manner that is understandable to scientists from diverse backgrounds. However, the journal generally does not publish highly specialized research.