富缺陷层状双氢氧化物介导的 CO2 还原和 5-HMF 氧化过程耦合,Dalton Transactions

当前位置： X-MOL 学术 › Dalton Trans. › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

富缺陷层状双氢氧化物介导的 CO2 还原和 5-HMF 氧化过程耦合
Dalton Transactions ( IF 3.5 ) Pub Date : 2023-01-12 , DOI: 10.1039/d2dt03886b
Jingjing Fan ₁ , Yin Zhao ₁ , Qian Wang ₁ , Mingyu Gao ₁ , Xintao Li ₁ , Dianqing Li _{1,

2} , Junting Feng _{1,

2}

Affiliation

针对废弃碳资源和可再生碳资源的综合利用，我们提出了层状双氢氧化物（LDHs）阴离子化合物介导的CO ₂还原和5-羟甲基糠醛（5-HMF）氧化的光催化偶联过程。具体而言，通过共沉淀法合成了 ZnNiFe–LDH，在此过程中，CO ₂以碳酸盐的形式储存在 LDH 层之间。^{然后，通过选择性蚀刻Zn 2+}，在LDH纳米片中引入一定量的金属空位离子。ICP-AES、EPR和XPS表明，随着刻蚀时间的延长，Zn空位浓度逐渐增加，从而优化了LDH层的电子结构。在富电子金属阳离子和层上羟基的催化下，层间碳酸盐被原位还原为CO，同时5-HMF氧化为2.5-呋喃二甲醛（DFF）。与未蚀刻的 ZnNiFe–LDHs 相比，在密度为 500 mW cm ^-2的紫外-可见光照射下，蚀刻 3 小时的 LDHs 的 CO 和 DFF 产率分别增加了 2.84 和 2.82 倍。最后，结合同位素标记的¹³ CO ₂实验和原位通过 FTIR 表征，我们揭示了可能的耦合机制和缺陷诱导的性能增强机制。

"点击查看英文标题和摘要"

Process coupling of CO2 reduction and 5-HMF oxidation mediated by defect-enriched layered double hydroxides

Aiming at the comprehensive utilization of waste carbon resources and renewable carbon resources, we put forward the photocatalytic coupling process of CO₂ reduction and 5-hydroxymethylfurfural (5-HMF) oxidation mediated by the anionic compound of layered double hydroxides (LDHs). Specifically, a ZnNiFe–LDH was synthesized by co-precipitation method, during which CO₂ was stored between LDH layers in the form of carbonate. Then, a certain amount of metal vacancies were introduced into LDH nanosheets by selectively etching Zn²⁺ ions. ICP-AES, EPR and XPS showed that the concentration of Zn vacancies gradually increased with the etching time prolonging, which thus optimized the electronic structure of LDH layers. Under the catalysis of the electron-rich metal cations and hydroxyl groups on the layers, the interlayer carbonate was in situ reduced into CO coupled accompanied with the 5-HMF oxidation to 2.5-furandiformaldehyde (DFF). Compared with the unetched ZnNiFe–LDHs, the CO and DFF yields over the LDHs etched for 3 h were increased by 2.84 and 2.82 times under UV-vis irradiation with a density of 500 mW cm⁻². Finally, combined with isotope-labeled ¹³CO₂ experiments and in situ FTIR characterization, we revealed the possible coupling mechanism and defect-induced performance enhancement mechanism.

更新日期：2023-01-12

点击分享查看原文

点击收藏

阅读更多本刊最新论文本刊介绍/投稿指南

全部期刊列表>>