通过 EDTA 接枝 UiO-66-NH2 的钴原子活性位点，在二氧化碳光还原过程中提高合成气产量

IF 5.4 3区材料科学 Q2 CHEMISTRY, PHYSICAL

ACS Applied Energy Materials Pub Date : 2024-09-18 DOI:10.1021/acsaem.4c01729

Toan-Anh Quach, Minh-Khoa Duong, Sakar Mohan, Trong-On Do

{"title":"通过 EDTA 接枝 UiO-66-NH2 的钴原子活性位点，在二氧化碳光还原过程中提高合成气产量","authors":"Toan-Anh Quach, Minh-Khoa Duong, Sakar Mohan, Trong-On Do","doi":"10.1021/acsaem.4c01729","DOIUrl":null,"url":null,"abstract":"In recent years, the use of photocatalysts has emerged as a promising research direction to transform harmful CO2 molecules into renewable fuels. In this work, the chelating agent ethylenediaminetetraacetic acid (EDTA) containing a central metal atom like Co was attached to the UiO-66-NH2 metal–organic frameworks (MOFs) through a one-pot synthesis. Several samples with different molar ratios of UiO-66-NH2–Co and EDTA (molar ratios of UiO-66-NH2–Co/EDTA is 1.2; 0.6; and 0.4) were synthesized and assessed for photocatalytic CO2 reduction to produce syngas (the mixture of CO and H2), which can be used for generating liquid fuels. Among these samples, the highest syngas production rate was achieved by sample U-E-0.6, yielding around 776.40 and 1217.29 μmol g–1 h–1 of CO and H2, respectively, at the end of 4 h. Multiple investigations, including electrochemical impedance, time-resolved, steady state photoluminescence, linear sweep voltammetry, and photocurrent measurements, revealed that the addition of EDTA-metal to UiO-66-NH2 improved the photoelectrochemical properties of the system, thereby enhancing its photocatalytic activity under solar irradiation. This research paves the way for the development of a single atom encapsulated in the MOF material for photocatalytic CO2 reduction.","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":null,"pages":null},"PeriodicalIF":5.4000,"publicationDate":"2024-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Cobalt-Atom Active Sites Grafted UiO-66-NH2 via EDTA for the Enhanced Production of Syngas in CO2 Photoreduction\",\"authors\":\"Toan-Anh Quach, Minh-Khoa Duong, Sakar Mohan, Trong-On Do\",\"doi\":\"10.1021/acsaem.4c01729\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"In recent years, the use of photocatalysts has emerged as a promising research direction to transform harmful CO2 molecules into renewable fuels. In this work, the chelating agent ethylenediaminetetraacetic acid (EDTA) containing a central metal atom like Co was attached to the UiO-66-NH2 metal–organic frameworks (MOFs) through a one-pot synthesis. Several samples with different molar ratios of UiO-66-NH2–Co and EDTA (molar ratios of UiO-66-NH2–Co/EDTA is 1.2; 0.6; and 0.4) were synthesized and assessed for photocatalytic CO2 reduction to produce syngas (the mixture of CO and H2), which can be used for generating liquid fuels. Among these samples, the highest syngas production rate was achieved by sample U-E-0.6, yielding around 776.40 and 1217.29 μmol g–1 h–1 of CO and H2, respectively, at the end of 4 h. Multiple investigations, including electrochemical impedance, time-resolved, steady state photoluminescence, linear sweep voltammetry, and photocurrent measurements, revealed that the addition of EDTA-metal to UiO-66-NH2 improved the photoelectrochemical properties of the system, thereby enhancing its photocatalytic activity under solar irradiation. This research paves the way for the development of a single atom encapsulated in the MOF material for photocatalytic CO2 reduction.\",\"PeriodicalId\":4,\"journal\":{\"name\":\"ACS Applied Energy Materials\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":5.4000,\"publicationDate\":\"2024-09-18\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Applied Energy Materials\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://doi.org/10.1021/acsaem.4c01729\",\"RegionNum\":3,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Applied Energy Materials","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1021/acsaem.4c01729","RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}

引用次数: 0

摘要

近年来，使用光催化剂将有害的二氧化碳分子转化为可再生燃料已成为一个前景广阔的研究方向。在这项研究中，通过一锅合成法将含有 Co 等中心金属原子的螯合剂乙二胺四乙酸（EDTA）连接到 UiO-66-NH2 金属有机框架（MOFs）上。合成了几种不同摩尔比的 UiO-66-NH2-Co 和 EDTA 样品（UiO-66-NH2-Co/EDTA 的摩尔比分别为 1.2、0.6 和 0.4），并对其进行了光催化还原 CO2 生成合成气（CO 和 H2 的混合物）的评估，合成气可用于生成液体燃料。在这些样品中，U-E-0.6 样品的合成气生产率最高，在 4 小时结束时分别产生了约 776.40 和 1217.29 μmol g-1 h-1 的 CO 和 H2。电化学阻抗、时间分辨、稳态光致发光、线性扫描伏安法和光电流测量等多项研究表明，在 UiO-66-NH2 中添加 EDTA 金属可改善该体系的光电化学特性，从而提高其在太阳光照射下的光催化活性。这项研究为开发封装在 MOF 材料中的单原子光催化还原 CO2 铺平了道路。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

Cobalt-Atom Active Sites Grafted UiO-66-NH2 via EDTA for the Enhanced Production of Syngas in CO2 Photoreduction

查看原文本刊更多论文

Cobalt-Atom Active Sites Grafted UiO-66-NH2 via EDTA for the Enhanced Production of Syngas in CO2 Photoreduction

In recent years, the use of photocatalysts has emerged as a promising research direction to transform harmful CO₂ molecules into renewable fuels. In this work, the chelating agent ethylenediaminetetraacetic acid (EDTA) containing a central metal atom like Co was attached to the UiO-66-NH₂ metal–organic frameworks (MOFs) through a one-pot synthesis. Several samples with different molar ratios of UiO-66-NH₂–Co and EDTA (molar ratios of UiO-66-NH₂–Co/EDTA is 1.2; 0.6; and 0.4) were synthesized and assessed for photocatalytic CO₂ reduction to produce syngas (the mixture of CO and H₂), which can be used for generating liquid fuels. Among these samples, the highest syngas production rate was achieved by sample U-E-0.6, yielding around 776.40 and 1217.29 μmol g^–1 h^–1 of CO and H₂, respectively, at the end of 4 h. Multiple investigations, including electrochemical impedance, time-resolved, steady state photoluminescence, linear sweep voltammetry, and photocurrent measurements, revealed that the addition of EDTA-metal to UiO-66-NH₂ improved the photoelectrochemical properties of the system, thereby enhancing its photocatalytic activity under solar irradiation. This research paves the way for the development of a single atom encapsulated in the MOF material for photocatalytic CO₂ reduction.

求助全文

通过发布文献求助，成功后即可免费获取论文全文。去求助

来源期刊

ACS Applied Energy Materials Materials Science-Materials Chemistry

CiteScore

10.30

自引率

6.20%

发文量

1368

期刊介绍： ACS Applied Energy Materials is an interdisciplinary journal publishing original research covering all aspects of materials, engineering, chemistry, physics and biology relevant to energy conversion and storage. The journal is devoted to reports of new and original experimental and theoretical research of an applied nature that integrate knowledge in the areas of materials, engineering, physics, bioscience, and chemistry into important energy applications.