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RISS 인기검색어
- 검색키워드
- 저자 : ZHOU HAORAN (검색결과 2 건)
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ZHOU HAORAN 고려대학교 대학원 2018 국내석사
Three Zn(II)–porphyrin sensitizers, coded as SGT-023, SGT-024 and SGT-025 were designed and synthesized through acceptor structural engineering. The photovoltaic performances of SGT sensitizer-based DSSCs were systematically evaluated with SGT-020 and SGT-021 as a reference sensitizer. The effect of the acceptor ability on photovoltaic performances was investigated for establishing the structure-performance relationship in the platform of D-π-A porphyrin sensitizers. By introducing a more planar acceptor unit in the porphyrin dyes, the power conversion efficiency (PCE) was reduced with the decreased short-circuit current (Jsc) and open-circuit voltage (Voc), due to the change of electron withdrawing ability in acceptor part. As a consequence, we obtained a maximum PCE of 5.6% for SGT-023, 4.2% for SGT-024 and 11.0% for SGT-025. To work out what was driving those differences, electrochemical impedance spectroscopy (EIS) and the time-resolved luminescence on Al2O3 and TiO2 film were measured to get insight into the electron injection dynamics of these five sensitizers. We have found that the dye with PTBA(SGT-023, SGT-024) and double ethynylene bridge (SGT-025) features a lower overall electron injection yield with respect to the dye with BTBA(SGT-020, SGT-021) owing to the sluggish electron injection and short lifetime of the excited state, accounting for a lower maximum of external quantum efficiencies of the device made from the dye with PTBA as an acceptor. Our studies have highlighted the importance of considering the excited state topology on the future design of low energy-gap photovoltaic materials.
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ZHOU HAORAN 고려대학교 대학원 2023 국내박사
본 학위논문은 신재생 대체에너지로 주목받고 있는 차세대 태양전지 중에서도 염료감응의 핵심 요소인 염료 및 공흡착 제의 개발을 위한 논문으로써, 기존 보고된 포피린 염료의 효 율을 능가하는 신규 포피린 염료를 개발과 동시에 포피린 염 료의 단점을 보완할 수 있는 공흡착제를 개발하고자, 새로운 전자주개 및 전자받개의 분자 설계 및 합성을 통하여 염료감 응 태양전지의 소자 성능 평가에 대한 연구를 보고하였다. 포피린은 넓게 동식물체에 존재하는 포르핀 유도체로 센서, 생리의학 및 에너지 분야에서 각광받고 있는 소재로, 염료감 응 태양전지 분야에서는 매우 높은 광전변환 효율을 나타내 는 것이다. 현재 보고되고 있는 고효율의 D-π-A 포피린 염료 의 구조는 전자 주개 그룹과 전자 받개 그룹을 포함하고 있 다. 기존의 포피린 염료보다 TiO2 흡착능력을 증가시키기 위 해, 전자받개에 기존 benzoic acid를salicylic acid 그룹으로 치 환하였고 포피린 염료 고유된 단점인 aggregation을 방지하 기 위해 긴 alky 사슬을 도입하여 소자 성능의 향상을 기대하 고자 하였다. 이에 따라 salicylic acid 그룹 함유된 SGT-028 및 긴 alky 사슬 함유된 SGT-029 포피린 염료를 합성 하였으며 이들을 염료 감응 태양 전지 소자에 적용하여 광-전 변환 특성을 분 석하였다. 그 결과, 더욱 강한 anchoring 그룹을 도입함으로써 장기 안정성이 높아졌으나 TiO2 흡착할때 더 tilt한 경향성이 나타났으며 긴 alky 사슬도 조금 더 낮은 흡착량을 초래하였 다. 결과에서는 광전류 값이 더 작게 나와서 광-전 변환 효율 이 떨어졌다. SGT-021의 전자주개인 BPFA (bis(7-(2,4- bis(hexyloxy)phenyl)-9,9-dimethyl-9H-fluoren-2-yl)amine)의 대 안으로서 비슷한 벌크구조를 가지는 Hex-BFPA (bis(4-(6,7- bis(hexyloxy)-9,9-dimethyl-9H-fluoren-2-yl)phenyl)amine) 와 BFPA (bis(4-(9,9-dihexyl-9H-fluoren-2-yl)phenyl)amine) 개발하 였고, 이를 도입한 신규염료 SGT-021(D)와 SGT-021(D0)를 개 발하였다. 합성적으로는 BPFA보다는 Hex-BFPA와 BFPA가 합 성루트가 더 짧으며 보다 더 높은 수율을 보여주어 생산비용 절감에 대한 장점이 있다. 하지만, BPFA에서 Hex-BFPA나 BFPA 전자주개로 교체하였을 경우에 흡광능력이 줄어들었다. 그 이유는 Hex-BFPA나 BFPA의 페닐기가 튀들리면서 말단의 플루오렌과 삼차아민간의 전자적 상호작용이 줄었기 때문으 로, 염료 전체의 콘쥬게이션 길이가 줄어들어 몰흡광계수가 감소하였을 뿐만 아니라 광흡수 대역도 좁아져 광감응능력이 대폭 감소하였기 때문이다. 소자제작 결과, SGT-021(D)의 광전 압만 높아졌으나 SGT-021(D)와 SGT-021(D0)가 SGT-021보다 감소된 광전류값을 보여주었다. 이는 BFPA의 뒤틀린 구조로 인한 흡광능력 저하가 효율 감소의 주된 원인이 되었다. 또한, 기존 많이 쓰였던 공합착제인 HC-A1 기반으로 전자 주개와 전자반개 설계를 통하여 HC-A6, HC-A7, HC-A8, HC-A9 와 HC-A10 총 5개 새로운 공합착제를 합성하였다. 이미 높은 광전 효율 달성한 염료인 SGT-021와 같이 TiO2에 공합착 시 켜 소자를 제작한 결과, HC-A7, HC-A9와 HC-A10는 포리린 염 료의 흡착량 감소에 이르게 되어서 광전류가 많이 떨어졌으 나 벌크 전자주개 가진 HC-A6가 가장 높은 효율을 달셩하였 다. 본 학위논문에서는 고효율 염료감응 태양전지용 염료의 분자설계 및 합성을 기반으로 소자특성평가를 통해 신규 염 료감응 태양전지를 개발하였고, 고효율용 포피린 염료와 공흡 착제의 분자 설계 및 합성시의 지침을 제시하였다. SGT-028 and SGT-029 are two porphyrin-based sensitizers that were created and manufactured using acceptor engineering for use in dye-sensitized solar cells (DSSCs). Instead of using a typical benzoic acid anchoring group, porphyrin SGT-028 was created by inserting a salicylic acid group. In SGT-029, the BTD was replaced with an extra alkylated benzothiadiazole (BTD) unit. SGT-021 was used as a reference dye. The result showed that the energy band gap and absorption range of these two porphyrin sensitizers were identical to those of the SGT-021 dye. SGT-029 had a power conversion efficiency (PCE) of 10.5% after DSSC devices had been optimized, although it was less effective than the benchmark porphyrin sensitizer SGT-021 (12.7%), while SGT-028 had a slightly lower PCE of 9.1% under the typical AM 1.5G light intensity. It should be noted that the PCE of 12.7% represents the best efficiency achieved by SGT-021. The dye adsorption amount discrepancy was cited as the primary cause since it might lead to the severe aggregate formation and reduced light harvest efficiency (LHE), which would reduce photocurrent, photovoltage, and PCE. As for donor engineering, two porphyrin-based sensitizers, SGT-021(D0) and SGT-021(D), were designed and synthesized via donor engineering for dye-sensitized solar cells (DSSCs). Fluorene-phenyl groups were introduced to both dyes, which have inversion structures in donor groups when compared with the platform of donor-porphyrin-triple bond-BTD-phenyl-acceptor sensitizer of SGT-021. Porphyrin SGT-021(D0) was designed by incorporating two hexyl chains into the 9-position of each fluorene. As for SGT-021(D), two hexyloxy chains unit was substituted to the terminal position of each fluorene in donor groups of porphyrin sensitizers. Both of these two donors could be synthesized by a much more facile route than SGT-021. The impact of the position of the long alkyl/alkoxyl chains on the optical and electrochemical properties and photovoltaic performance was studied and compared with a reference dye of SGT-021, which had previously been reported by our group. As a result, both porphyrin sensitizers obtained a similar absorption range and energy band gap to SGT-021 dye. After performing optimization of DSSC devices, SGT-021(D) achieved a comparatively high-power conversion efficiency (PCE) of 11.63%, and a slightly lower PCE of 10.5% was exhibited by SGT-021(D0), under the standard AM 1.5G light intensity. The performance of porphyrin-sensitized solar cells also could be enhanced by the structural modification of co-adsorbents. In this point of view, five novel co-adsorbents based on donor and acceptor engineering were also designed and synthesized. They were co-adsorbed with SGT-021 porphyrin dye for application in dye-sensitized solar cells (DSSCs), which has proved to be an efficient method to achieve efficiency. For comparison, the HC-A1adsorbents developed by our group previously were used as a reference co-adsorbent. Results from EIS, UV, electronic chemistry, and highest occupied molecular orbital−lowest unoccupied molecular orbital band gap calculations from density functional theory were analyzed to figure out the mechanistic way of our device. As a result, the highest efficiency of 12.25% was achieved by HC-A6-based DSSCs. It could be ascribed as the bulky rigid donor of HC-A6 would retard the charge recombination and enhance the light-harvesting properties.
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