Development of a Chemical Solution Method to Improve the Photoelectrochemical Hydrogen Production Performance of Antimony Sulfide (Sb₂S₃) Photoelectrode
- 주제(키워드) Antimony sulfide , TiO₂ bottom layer , chemical solution method , rapid thermal annealing , photoelectrochemical water splitting , iodide oxidation reaction
- 주제(DDC) 621.042
- 발행기관 아주대학교 일반대학원
- 지도교수 조인선
- 발행년도 2024
- 학위수여년월 2024. 2
- 학위명 석사
- 학과 및 전공 일반대학원 에너지시스템학과
- 실제URI http://www.dcollection.net/handler/ajou/000000033477
- 본문언어 영어
- 저작권 아주대학교 논문은 저작권에 의해 보호받습니다.
초록/요약
Global energy consumption is increasing as the world's population and industries expand. Photoelectrochemical hydrogen production holds great potential to solve the energy crisis and achieve the goal of carbon neutrality. Fabrication of highly efficient photoanode via cost effective method remains key challenges. Herein, we utilized a chemical solution method and rapid thermal annealing (RTA) process fabricated an efficient antimony sulfide (Sb₂S₃) photoanode. We showed that the TiO₂ bottom layer holds the key role in the Sb₂S₃ film formation and properties. By adjusting the TiO₂ bottom layer, we are able to synthesize a high uniformity and coverage Sb₂S₃ film with excellent light absorption ability. Besides, the RTA process can facilitate the Sb₂S₃ phase growth and formation, generating a high quality Sb₂S₃ film with large grain and crystallite size. The RTA annealed sample exhibits highest photocurrent density compared to other annealing method, which shows the high effectiveness of RTA methods. As a result, fabricated Sb₂S₃ photoanode showing a high photocurrent density of 3.2 mA/cm² at 1.23 V vs. RHE, which is one of the highest values among all reported Sb₂S₃ photoanode (without OEC and protection layer). Furthermore, we demonstrated an iodide oxidation reaction (IOR) to replace the sluggish OER to show the effectiveness of our Sb₂S₃ photoanode. Interestingly, we achieved a highest photocurrent density value of 7.7 mA/cm² at 0.6 V vs. RHE. Our work provides a cost-effective method for fabricating high efficiency Sb₂S₃ photoanode, paving the way for developing highly active sulfide based photoanode in the future.
more목차
1. Introduction 1
1.1 Energy crisis and carbon neutralization 1
1.2 Hydrogen as an ideal energy carrier 2
1.3 Photoelectrochemical (PEC) water splitting 3
1.4 Common materials for PEC water splitting 4
1.5 Sb₂S₃ as a photoanode for PEC water splitting 5
2. Experimental section 6
2.1 Materials 6
2.2 Synthesis of TiO₂ bottom buffer layer 7
2.3 TiCl₃ treatment for surface activation 7
2.4 Hydrothermal growth of Sb₂S₃ film 8
2.5 Annealing of Sb₂S₃ film 9
2.6 Material characterizations 10
2.7 (Photo)electrochemical measurements 12
3. Result and discussion 14
3.1 TiO₂ bottom layer effect on the Sb₂S₃ (SbS) film growth 14
3.1.1 TiO₂ bottom layer effect on the SbS film morphology 14
3.1.2 TiO₂ bottom layer effect on the optical property of SbS film 17
3.1.3 TiO₂ bottom layer effect on the SbS crystal phase & surface composition 19
3.2 Hydrothermal condition optimization 22
3.2.1 Growth time effect on film thickness 22
3.2.2 Growth time optimization 22
3.3 RTA temperature effect on the Sb₂S₃ film formation 25
3.3.1 RTA temperature effect on the morphology & phase formation 25
3.3.2 RTA temperature effect on the surface composition & chemical states 28
3.4 RTA and other annealing method comparison 30
3.4.1 RTA and other annealing method effect on the morphology 30
3.4.2 RTA and other annealing method effect on the phase formation & surface chemical states 32
3.5 (Photo)electrochemical performance and characterizations 34
3.5.1 TiO₂ bottom layer effect on the PEC performance 34
3.5.2 TiO₂ bottom layer effect on the charge dynamics and active sites 37
3.5.3 RTA temperature effect on the PEC performance 43
3.5.4 RTA temperature effect on the active sites, carrier concentrations 45
3.5.5 Different annealing method effect on the PEC performance 49
3.6 PEC iodide oxidation coupling with hydrogen production 51
4. Conclusion 55
5. Reference 56
국문 요약 62
