Anna Pancielejko, Mateusz A Baluk, Hanna Zagórska, Magdalena Miodyńska-Melzer, Anna Gołąbiewska, Tomasz Klimczuk, Mirosław Krawczyk, Mirosława Pawlyta, Krzysztof Matus, Alicja Mikolajczyk, Henry P Pinto, Aleksandra Pieczyńska, Joanna Dołżonek, Adriana Zaleska-Medynska
{"title":"铜掺杂的 NH2-MIL-125(Ti):增强光催化 H2 生成和 CO2 光转化的多功能可见光驱动平台。","authors":"Anna Pancielejko, Mateusz A Baluk, Hanna Zagórska, Magdalena Miodyńska-Melzer, Anna Gołąbiewska, Tomasz Klimczuk, Mirosław Krawczyk, Mirosława Pawlyta, Krzysztof Matus, Alicja Mikolajczyk, Henry P Pinto, Aleksandra Pieczyńska, Joanna Dołżonek, Adriana Zaleska-Medynska","doi":"10.1039/d4mh01116c","DOIUrl":null,"url":null,"abstract":"<p><p>Here, we present for the first time an efficient platform for simultaneous H<sub>2</sub> generation and CO<sub>2</sub> conversion into HCOOH, utilizing a Cu-incorporated NH<sub>2</sub>-MIL-125(Ti) material with triethanolamine as the sacrificial agent. When subjected to light, Cu-NH<sub>2</sub>-MIL-125(Ti) exhibits a remarkable enhancement in H<sub>2</sub> generation, with a 30-fold increase under UV-Vis light and an 8-fold increase under visible irradiation compared to the pristine MOF. The study on the CO<sub>2</sub> photoreduction ability of Cu-NH<sub>2</sub>-MIL-125(Ti) indicated successful conversion into formic acid yielding 62.4 μmol g<sub>cat</sub><sup>-1</sup> under visible irradiation. This notable improvement in photocatalytic activity can be attributed to the heightened light absorption capacity and efficient charge transportation and separation mechanisms inherent in Cu-NH<sub>2</sub>-MIL-125(Ti). Furthermore, the stability of the Cu-NH<sub>2</sub>-MIL-125(Ti) photocatalyst remains steady even after 24 hours of continuous irradiation. The theoretical simulations suggest that Cu introduction effectively reduces the bandgap while leaving the position and composition of the valence band unaffected.</p>","PeriodicalId":87,"journal":{"name":"Materials Horizons","volume":" ","pages":""},"PeriodicalIF":12.2000,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Cu-incorporated NH<sub>2</sub>-MIL-125(Ti): a versatile visible-light-driven platform for enhanced photocatalytic H<sub>2</sub> generation and CO<sub>2</sub> photoconversion.\",\"authors\":\"Anna Pancielejko, Mateusz A Baluk, Hanna Zagórska, Magdalena Miodyńska-Melzer, Anna Gołąbiewska, Tomasz Klimczuk, Mirosław Krawczyk, Mirosława Pawlyta, Krzysztof Matus, Alicja Mikolajczyk, Henry P Pinto, Aleksandra Pieczyńska, Joanna Dołżonek, Adriana Zaleska-Medynska\",\"doi\":\"10.1039/d4mh01116c\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p><p>Here, we present for the first time an efficient platform for simultaneous H<sub>2</sub> generation and CO<sub>2</sub> conversion into HCOOH, utilizing a Cu-incorporated NH<sub>2</sub>-MIL-125(Ti) material with triethanolamine as the sacrificial agent. When subjected to light, Cu-NH<sub>2</sub>-MIL-125(Ti) exhibits a remarkable enhancement in H<sub>2</sub> generation, with a 30-fold increase under UV-Vis light and an 8-fold increase under visible irradiation compared to the pristine MOF. The study on the CO<sub>2</sub> photoreduction ability of Cu-NH<sub>2</sub>-MIL-125(Ti) indicated successful conversion into formic acid yielding 62.4 μmol g<sub>cat</sub><sup>-1</sup> under visible irradiation. This notable improvement in photocatalytic activity can be attributed to the heightened light absorption capacity and efficient charge transportation and separation mechanisms inherent in Cu-NH<sub>2</sub>-MIL-125(Ti). Furthermore, the stability of the Cu-NH<sub>2</sub>-MIL-125(Ti) photocatalyst remains steady even after 24 hours of continuous irradiation. The theoretical simulations suggest that Cu introduction effectively reduces the bandgap while leaving the position and composition of the valence band unaffected.</p>\",\"PeriodicalId\":87,\"journal\":{\"name\":\"Materials Horizons\",\"volume\":\" \",\"pages\":\"\"},\"PeriodicalIF\":12.2000,\"publicationDate\":\"2024-11-15\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Materials Horizons\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://doi.org/10.1039/d4mh01116c\",\"RegionNum\":2,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Materials Horizons","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1039/d4mh01116c","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
摘要
在这里,我们首次利用以三乙醇胺为牺牲剂的 Cu 嵌入 NH2-MIL-125(Ti)材料,提出了一种同时生成 H2 和将 CO2 转化为 HCOOH 的高效平台。与原始 MOF 相比,Cu-NH2-MIL-125(Ti) 在光照下生成 H2 的能力显著提高,在紫外可见光下提高了 30 倍,在可见光照射下提高了 8 倍。对 Cu-NH2-MIL-125(Ti) CO2 光还原能力的研究表明,在可见光照射下,它能成功地将 CO2 转化为甲酸,产生 62.4 μmol gcat-1。光催化活性的显著提高可归因于 Cu-NH2-MIL-125(Ti) 所固有的更强的光吸收能力以及高效的电荷传输和分离机制。此外,Cu-NH2-MIL-125(Ti) 光催化剂的稳定性在连续照射 24 小时后仍能保持稳定。理论模拟表明,铜的引入有效地减小了带隙,同时价带的位置和组成未受影响。
Cu-incorporated NH2-MIL-125(Ti): a versatile visible-light-driven platform for enhanced photocatalytic H2 generation and CO2 photoconversion.
Here, we present for the first time an efficient platform for simultaneous H2 generation and CO2 conversion into HCOOH, utilizing a Cu-incorporated NH2-MIL-125(Ti) material with triethanolamine as the sacrificial agent. When subjected to light, Cu-NH2-MIL-125(Ti) exhibits a remarkable enhancement in H2 generation, with a 30-fold increase under UV-Vis light and an 8-fold increase under visible irradiation compared to the pristine MOF. The study on the CO2 photoreduction ability of Cu-NH2-MIL-125(Ti) indicated successful conversion into formic acid yielding 62.4 μmol gcat-1 under visible irradiation. This notable improvement in photocatalytic activity can be attributed to the heightened light absorption capacity and efficient charge transportation and separation mechanisms inherent in Cu-NH2-MIL-125(Ti). Furthermore, the stability of the Cu-NH2-MIL-125(Ti) photocatalyst remains steady even after 24 hours of continuous irradiation. The theoretical simulations suggest that Cu introduction effectively reduces the bandgap while leaving the position and composition of the valence band unaffected.