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Investigation of Cyanide-Based Catalysts and Hybrid Assemblies for Artificial Photosynthesis = = Yapay Fotosentez Icin Siyanur Bazli Katalizorler ve Hibrit Duzenlemelerin Incelenmesi.

紀錄類型:	書目-電子資源 : Monograph/item
正題名/作者:	Investigation of Cyanide-Based Catalysts and Hybrid Assemblies for Artificial Photosynthesis =/
其他題名:	Yapay Fotosentez Icin Siyanur Bazli Katalizorler ve Hibrit Duzenlemelerin Incelenmesi.
其他題名:	Yapay Fotosentez Icin Siyanur Bazli Katalizorler ve Hibrit Duzenlemelerin Incelenmesi.
作者:	Akbari, Sina Sadigh.
面頁冊數:	1 online resource (183 pages)
附註:	Source: Dissertations Abstracts International, Volume: 84-05, Section: B.
Contained By:	Dissertations Abstracts International84-05B.
標題:	Solar energy. -
電子資源:	http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=30158245click for full text (PQDT)
ISBN:	9798352987100

Investigation of Cyanide-Based Catalysts and Hybrid Assemblies for Artificial Photosynthesis = = Yapay Fotosentez Icin Siyanur Bazli Katalizorler ve Hibrit Duzenlemelerin Incelenmesi.
Akbari, Sina Sadigh.

Investigation of Cyanide-Based Catalysts and Hybrid Assemblies for Artificial Photosynthesis =Yapay Fotosentez Icin Siyanur Bazli Katalizorler ve Hibrit Duzenlemelerin Incelenmesi.Yapay Fotosentez Icin Siyanur Bazli Katalizorler ve Hibrit Duzenlemelerin Incelenmesi. - 1 online resource (183 pages)

Source: Dissertations Abstracts International, Volume: 84-05, Section: B.

Thesis (Ph.D.)--Bilkent Universitesi (Turkey), 2022.

Includes bibliographical references

The storage and conversion of solar energy appear to be a highly promising solution to the global energy dilemma due to the sustainability and abundance of sunlight. Among various strategies, artificial photosynthesis, in which solar energy is directly converted to chemical bonds, has gained a great deal of attraction over the past decades. Such a design requires a catalyst coupled with a semiconductor and/or a photosensitizer as light-harvesting components with proper band levels for efficient charge separation. Therefore, the development of an earth-abundant, robust, and visible-light absorbing photocatalytic assembly has been one of the bottlenecks for the advancement of scalable cells. This work aims to overcome this critical challenge by developing new cyanide-based hybrid assemblies for light-driven water splitting and CO2 reduction.CoFe Prussian blue analogues (CoFe-PBAs) have recently emerged as active water oxidation catalysts with excellent long-term stabilities. In the first study, a ZnCr layered double hydroxide (ZnCr-LDH) with a two-dimensional (2D) morphology and a CoFe-PBA are combined to afford a precious metal-free photocatalytic assembly involving a visible light-absorbing semiconductor (SC) and a water oxidation catalyst (WOC). The SC−WOC hybrid materials exhibit a threefold enhancement in activity compared to bare ZnCr-LDH, which is maintained for 6 h under photocatalytic conditions. The band energy diagram was extracted from optical and electrochemical studies to clarify the origin of the improved photocatalytic performance. The assembly is observed to have an appropriate band energy alignment that facilitates charge transfer from the valence band of ZnCr-LDH to the HOMO level of CoFe-PBA for the water oxidation process. In a follow-up study, we move one step forward by coupling exfoliated Dion−Jacobson type niobate nanosheets as a 2D semiconductor with the CoFe-PBA to construct an SC−WOC hybrid structure, which produces a p−n junction. The assembly exhibits a promoted activity (89.5 μmol g−1 h−1) with a proper band energy alignment for the photocatalytic water oxidation process, and it is stable throughout a 12 h photocatalytic study. These studies mark a straightforward pathway to developing low-cost and precious metal-free assemblies for light-driven water oxidation.Metal dicyanamides are another well-known cyanide-based materials, which can be employed as a catalyst for hydrogen evolution reaction (HER) and CO2 reduction due to the partial electron delocalization and the proper coordination environment of metal ions. Herein, we promote a cobalt dicyanamide coordination polymer, Co-dca, for the first time, as a selective catalyst to reduce CO2 to CO in the presence of a ruthenium photosensitizer (Ru PS) under visible light irradiation. A series of photocatalytic experiments under various reaction conditions were performed to reveal the role of the PS, the scavenger, and the solvent in the selectivity and the activity of the photocatalytic process. We find that Co-dca exhibits an activity of 254 µmol h−1 g−1 and a CO selectivity as high as 93%. Furthermore, cobalt dicyanamide also displayed enhanced H2 evolution activity (25000 µmol h−1 g−1), which is maintained for at least 12 h in a mixed aqueous solution containing a Ru-based photosensitizer and a sacrificial electron donor. The effect of various reaction parameters on the photocatalytic activity of the system was investigated.Overall, this thesis presents various low-cost and stable SC-WOC hybrid assemblies based on CoFe-PBA for the light-driven water oxidation process. Moreover, we suggest the use of Co-dca, for the first time, as catalysts for HER and CO2 reduction reactions.

Electronic reproduction.
Ann Arbor, Mich. :
ProQuest,
2023

Mode of access: World Wide Web

ISBN: 9798352987100Subjects--Topical Terms:

520346
Solar energy.
Index Terms--Genre/Form:

542853
Electronic books.

Investigation of Cyanide-Based Catalysts and Hybrid Assemblies for Artificial Photosynthesis = = Yapay Fotosentez Icin Siyanur Bazli Katalizorler ve Hibrit Duzenlemelerin Incelenmesi.
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504 $a Includes bibliographical references
520 $a The storage and conversion of solar energy appear to be a highly promising solution to the global energy dilemma due to the sustainability and abundance of sunlight. Among various strategies, artificial photosynthesis, in which solar energy is directly converted to chemical bonds, has gained a great deal of attraction over the past decades. Such a design requires a catalyst coupled with a semiconductor and/or a photosensitizer as light-harvesting components with proper band levels for efficient charge separation. Therefore, the development of an earth-abundant, robust, and visible-light absorbing photocatalytic assembly has been one of the bottlenecks for the advancement of scalable cells. This work aims to overcome this critical challenge by developing new cyanide-based hybrid assemblies for light-driven water splitting and CO2 reduction.CoFe Prussian blue analogues (CoFe-PBAs) have recently emerged as active water oxidation catalysts with excellent long-term stabilities. In the first study, a ZnCr layered double hydroxide (ZnCr-LDH) with a two-dimensional (2D) morphology and a CoFe-PBA are combined to afford a precious metal-free photocatalytic assembly involving a visible light-absorbing semiconductor (SC) and a water oxidation catalyst (WOC). The SC−WOC hybrid materials exhibit a threefold enhancement in activity compared to bare ZnCr-LDH, which is maintained for 6 h under photocatalytic conditions. The band energy diagram was extracted from optical and electrochemical studies to clarify the origin of the improved photocatalytic performance. The assembly is observed to have an appropriate band energy alignment that facilitates charge transfer from the valence band of ZnCr-LDH to the HOMO level of CoFe-PBA for the water oxidation process. In a follow-up study, we move one step forward by coupling exfoliated Dion−Jacobson type niobate nanosheets as a 2D semiconductor with the CoFe-PBA to construct an SC−WOC hybrid structure, which produces a p−n junction. The assembly exhibits a promoted activity (89.5 μmol g−1 h−1) with a proper band energy alignment for the photocatalytic water oxidation process, and it is stable throughout a 12 h photocatalytic study. These studies mark a straightforward pathway to developing low-cost and precious metal-free assemblies for light-driven water oxidation.Metal dicyanamides are another well-known cyanide-based materials, which can be employed as a catalyst for hydrogen evolution reaction (HER) and CO2 reduction due to the partial electron delocalization and the proper coordination environment of metal ions. Herein, we promote a cobalt dicyanamide coordination polymer, Co-dca, for the first time, as a selective catalyst to reduce CO2 to CO in the presence of a ruthenium photosensitizer (Ru PS) under visible light irradiation. A series of photocatalytic experiments under various reaction conditions were performed to reveal the role of the PS, the scavenger, and the solvent in the selectivity and the activity of the photocatalytic process. We find that Co-dca exhibits an activity of 254 µmol h−1 g−1 and a CO selectivity as high as 93%. Furthermore, cobalt dicyanamide also displayed enhanced H2 evolution activity (25000 µmol h−1 g−1), which is maintained for at least 12 h in a mixed aqueous solution containing a Ru-based photosensitizer and a sacrificial electron donor. The effect of various reaction parameters on the photocatalytic activity of the system was investigated.Overall, this thesis presents various low-cost and stable SC-WOC hybrid assemblies based on CoFe-PBA for the light-driven water oxidation process. Moreover, we suggest the use of Co-dca, for the first time, as catalysts for HER and CO2 reduction reactions.
520 $a Gunes enerjisinin depolanmasi ve donusturulmesi, gunes isiginin surdurulebilirligi ve bollugu nedeniyle kuresel enerji icin oldukca umut verici bir cozum olarak kabul edilmektedir. Cesitli stratejiler arasinda, gunes enerjisinin dogrudan kimyasal baglara donusturuldugu yapay fotosentez, gectigimiz yillarda buyuk bir ilgi gordu. Boyle bir tasarim, verimli yuk ayrimi icin uygun bant seviyelerine sahip bir yari iletken ve/veya isiga duyarli bir malzeme ile birlestirilmis bir katalizor gerektirmektedir. Bu nedenle, yeryuzunde bol, saglam ve gorunur isik soguran bir fotokatalitik duzenegin gelistirilmesi, olceklenebilir hucrelerin ilerlemesi icin en zor adim olmustur. Bu calisma, fotokatalitik yontemle hidrojen olusturma ve CO2 indirgemesi icin yeni siyanur temelli hibrit duzenekler gelistirerek bu kritik zorlugun ustesinden gelmeyi amaclamaktadir.Yapilan calismalar, CoFe Prusya mavisi analoglarinin (CoFe-PBA) mukemmel uzun vadeli kararliliklara sahip aktif su oksidasyon katalizorleri oldugunu gostermektedir. Bu tezdeki ilk calisma, iki boyutlu (2D) morfolojiye sahip tabakali bir cift hidroksit (ZnCrLDH) bilesikle bir CoFe-PBA yapisinin birlestirilerek degerli metal icermeyen fotokatalitik bir duzenek gelistirilmesi uzerinedir. SC−WOC hibrit malzemeleri, fotokatalitik kosullar altinda 6 saat boyunca kararli kalmakla birlikte, ZnCr-LDH'ye kiyasla aktivitede uc kat bir artis sergiler. Fotokatalitik performansin kaynagini anlamak icin optik ve elektrokimyasal calismalar yardimiyla bant enerji diyagrami ortaya cikarilmistir. Duzenegin, su oksidasyon islemi icin ZnCr-LDH valans bandindan CoFe-PBAnin HOMO seviyesine yuk transferini kolaylastiran uygun bir bant enerji diyagramina sahip oldugu gozlemlenmistir.Bunu takip eden calismada, bir p-n junction ureten bir SC-WOC hibrit yapisi olusturmak icin 2D yari iletken exfole edilmis Dion-Jacobson tipi niyobat nano tabakalarini CoFe-PBA ile birlestirerek bir adim ileri gidiyoruz. Hibrit malzeme fotokatalitik yontemle suyun yukseltgenmesi islemi icin uygun bir bant enerji seviyesi yardimiyla yuksek bir aktivite (89,5 μmol g−1 h −1) sergilemektedir ve 12 saatlik bir fotokatalitik calisma boyunca kararlidir. Bu calismalar, isikla su oksidasyonu icin dusuk maliyetli ve degerli metal icermeyen duzenekler gelistirmeye yonelik basit bir yolu isaret ediyor.Metal disyanamitler, kismi elektron delokalizasyonu ve metal iyonlarinin uygun koordinasyon ortami nedeniyle hidrojen olusumu reaksiyonu (HER) ve CO2 indirgemesi icin bir katalizor olarak kullanilabilecek diger iyi bilinen siyanur temelli malzemelerdir. Burada, gorunur isiga duyarli bir rutenyum bilesigi (Ru PS) varliginda CO2'yi CO'ya indirgemek icin secici bir katalizor olarak ilk kez bir kobalt disyanamit koordinasyon polimeri olan Co-dca'yi kullandik. Co-dca'nin 254 µmol h−1 g −1 aktivite ve %93 kadar yuksek bir CO seciciligi sergiledigini bulduk. Ayrica, kobalt disyanamit, sulu bir cozeltide en az 12 saat surdurulen H2 olusturma aktivitesi (25000 µmol h−1 g −1) sergilemektedir. Fotokatalitik prosesin seciciligi ve etkinliginde PS'nin, elektron donoru ve cozucunun rolunu ortaya cikarmak icin cesitli reaksiyon kosullari altinda bir dizi fotokatalitik deney yapildi. Sistemin fotokatalitik aktivitesi uzerine cesitli reaksiyon parametrelerinin etkisi arastirildi.
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