Highly Selective Photoreduction of CO<sub>2</sub> with Suppressing H<sub>2</sub> Evolution over Monolayer Layered Double Hydroxide under Irradiation above 600 nm

Tan, Ling; Xu, Sen; Wang, Zelin; Xu, Yanqi; Wang, Xian; Hao, Xihong; Bai, Sha; Ning, Chenjun; Wang, Yu; Zhang, Wenkai; Jo, Young‐Heon; Hwang, Seong Ju; Cao, Xingzhong; Zheng, Xusheng; Yan, Hong; Zhao, Yufei; Duan, Haohong; Song, Yu

doi:10.1002/anie.201904246

Cited by 253 publications

(142 citation statements)

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“…Tan and co-workers developed a monolayer NiAl-LDH for selective photoreduction of CO 2 and H 2 O into CH 4 and CO and achieved completely suppressed H 2 evolution reaction under irradiation with λ > 600 nm as reveal by 13 CO 2 isotope labeling, activity reaction under different wavelengths. [90] In conclusion, XAFS, XAS, and PAS results confirmed the introduction of ample coordinately unsaturated metal and hydroxyl defects in NiAl-LDH. Spin-polarized DFT + U calculations (in Figure 18a-c) illuminated that the Gibbs free energy barrier of CO 2 reduction to CH 4 greatly decreased from 0.486 eV to 0.127 eV because of the synergistic effect of metal and hydroxyl defects in m-NiAl-LDH.…”

Section: Co 2 Activation Via Vacanciesmentioning

confidence: 53%

Role of Vacancies in Photocatalysis: A Review of Recent Progress

Zhang

et al. 2020

Chemistry An Asian Journal

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Photocatalysis via direct solar-to-chemical energy conversion is an intriguing approach for alleviating the pressure of high energy consumption caused by social development. However, photocatalytic efficiency is greatly restricted by unsatisfactory light-harvesting capacity, high carrier recombination rates, and sluggish reaction kinetics. Indeed, vacancy engineering is an attractive strategy to regulate photocatalytic reaction performance to maximize the utilization and storage of solar energy. In this review, we summarize recent progress about the important roles of vacancy defects on solar-driven photocatalytic applications. The current advanced characterization techniques, especially for in situ/operando techniques, are first presented for elucidating the structure-performance relationships of defective semiconductors in photocatalysis. Subsequently, the crucial roles of vacancies in enhancing photocatalytic performance are highlighted from three important processes: light absorption, carrier separation and migration, and surface reaction. Finally, based on the above understanding, perspectives and opportunities about defective materials are considered for various photocatalytic applications.

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Section: Co 2 Activation Via Vacanciesmentioning

confidence: 53%

Role of Vacancies in Photocatalysis: A Review of Recent Progress

Zhang

et al. 2020

Chemistry An Asian Journal

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“…Moreover, as shown from AFM results (Figure 1f-g), the thickness of m-NiAl-LDH was 1 nm, in accordance with TEM and HRTEM results. [11] Such characterization clearly observed the morphology of nanostructured LDH, provided a detailed information for the further photocatalysis. In 2017, Xie and co-workers synthesized a β-Ni (OH) 2 ultrathin nanomeshes with amount of nanopores by etching-intralayered Ostwald ripening NiAl-LDH ( Figure 1h).…”

Section: Morphology and Compositionmentioning

confidence: 86%

“…[9b] In nanomeshes. [11][12] addition, such a rational design of photocatalytic LDHs-based materials resulted in the suitable bandgap, which allowed the possible excitation under visible light irradiation, provided a tunable redox potential for the further reduction reaction (CO 2 reduction, [13] N 2 fixation [14] etc.) or oxidation process (water oxidation, [15] oxidation of benzene [16] etc.).…”

Section: Morphology and Compositionmentioning

confidence: 99%

“…Furthermore, ascribing to the virtue properties of metal-to-metal charge transfer (MMCT) and metalto-ligand charge transfer (MLCT), transition metal containing -LDHs performed efficient photocatalytic activity under much longer wavelength (such as: λ > 600 nm) irradiation, further enhance the utilization of solar energy. [11,18] By taking full use of these virtue advantages of LDHs-based photocatalysts, researchers have attempted various strategies to promote the photocatalytic selectivity of CO 2 PR. LDHs was firstly reported as photocatalysts for CO 2 PR by Izumi et al in 2011.…”

Section: Morphology and Compositionmentioning

confidence: 99%

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Recent Progress on Nanostructured Layered Double Hydroxides for Visible‐Light‐Induced Photoreduction of CO₂

Tan

Wang

Zhao

et al. 2020

Chemistry An Asian Journal

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Photoreduction of CO 2 into solar fuels is usually regarded as one of the promising solutions to overcome environmental pollution and the energy crisis. The main challenge in CO 2 photoreduction (CO 2 PR) is the low efficiency and poor selectivity. Layered double hydroxides (LDHs) are a class of 2D materials, consisting with M(OH) 6 octahedra in the host layers and intercalated anions. Owing to the tuneable composition, particle size, morphology, and virtue coordinatively unsaturated active sites, a series of efficient strategies (morphology control, heterostructure, defect control, etc.) in LDH-based photocatalysts have been efficiently developed to enhance the photocatalytic selectivity and activity for CO 2 PR. This review summarizes recent progress on the LDH-based photocatalysts for CO 2 PR. Al 3 + and transition metal elements, Fe 2 + , Co 2 + , Ni 2 + , Zn 2 + , Cr 3 + , Fe 3 + , etc.) in the laminate layers and A nÀ is the interlaminated anion (such as: NO 3 À , CO 3 2À and SO 4 2À , etc.) in the interlayer. [6b,c,7] It has been widely applied in photocatalyst in the past decades. [8] Ascribe to the tunable atomic structure, the bandgap of LDHs can be tuned from 2.0 eV to 5.4 eV by changing the composition of layer. [9] Moreover, the surface defects (such as: V M , metal vacancy and V OH , hydroxyl vacancy, etc.) as active sites in photocatalysis can be easily introduced by controlling the thickness and size of LDHs etc., thus promoting the efficiency of CO 2 PR. This review focuses on the recent development of the LDHs-based photocatalysts for CO 2 PR, and the corresponding progress of CO 2 PR has achieved great progress from the former CO 2 conversion rate of~1 μmol g À 1 h À 1 to recent 218130 μmol g À 1 h À 1 , and the desirable valuable-product also move from CO to CH 4 and methanol. The major strategies of promoting the CO 2 PR are discussed from different perspective from the morphology and composition, electronic structure, and defects structure for further understanding the relationship between the structure and activity.

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“…2À or Cl À ), and z is the amount of water. [41] It is well-known that they have been utilized in several application, for example, adsorption, [42] drug delivery, [43] and especially catalysis including photocatalytic reaction, [44,45] water splitting, [46] CO 2 reduction [47,48] and acid-base reactions. [49,50] Recently, not only the hybrid zeolite@LDH has been fabricated, but also the transformation of coated LDH to metal oxides deposited on external surfaces of zeolite is an interesting perspective in catalysis.…”

Section: Introductionmentioning

confidence: 99%

Modified Acid‐Base ZSM‐5 Derived from Core‐Shell ZSM‐5@ Aqueous Miscible Organic‐Layered Double Hydroxides for Catalytic Cracking of n‐Pentane to Light Olefins

et al. 2020

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Over the past decades, the catalytic cracking catalysts for hydrocarbon oil upgrading have been extensively developed to increase the yield of light olefins. In this context, we report the fabrication of the core‐shell ZSM‐5@aqueous miscible organic‐layered double hydroxides prepared by the growth of layered double hydroxides (LDH) precursors on zeolite surfaces. The deposited LDH results in a decrease of the number of strong Brønsted acid sites on zeolite surfaces and its transformation at high temperature leads to produce the highly dispersed metal oxides deposited on external surfaces of zeolites. Therefore, the acid‐base properties of designed surfaces are modified, eventually resulting in the suppression of competing hydride transfers and further side reactions. As a result, there is a significant enhancement in light olefins production compared with the pristine zeolite. In addition, the designed catalysts exhibit high recycling stability and reusability. This first example opens up the new perspectives for the development of modified acid‐base zeolites using zeolite@aqueous miscible organic‐layered double hydroxides for the catalytic upgrading of hydrocarbons.

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Highly Selective Photoreduction of CO₂ with Suppressing H₂ Evolution over Monolayer Layered Double Hydroxide under Irradiation above 600 nm

Cited by 253 publications

References 56 publications

Role of Vacancies in Photocatalysis: A Review of Recent Progress

Role of Vacancies in Photocatalysis: A Review of Recent Progress

Recent Progress on Nanostructured Layered Double Hydroxides for Visible‐Light‐Induced Photoreduction of CO₂

Modified Acid‐Base ZSM‐5 Derived from Core‐Shell ZSM‐5@ Aqueous Miscible Organic‐Layered Double Hydroxides for Catalytic Cracking of n‐Pentane to Light Olefins

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Highly Selective Photoreduction of CO2 with Suppressing H2 Evolution over Monolayer Layered Double Hydroxide under Irradiation above 600 nm

Cited by 253 publications

References 56 publications

Role of Vacancies in Photocatalysis: A Review of Recent Progress

Role of Vacancies in Photocatalysis: A Review of Recent Progress

Recent Progress on Nanostructured Layered Double Hydroxides for Visible‐Light‐Induced Photoreduction of CO2

Modified Acid‐Base ZSM‐5 Derived from Core‐Shell ZSM‐5@ Aqueous Miscible Organic‐Layered Double Hydroxides for Catalytic Cracking of n‐Pentane to Light Olefins

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Highly Selective Photoreduction of CO₂ with Suppressing H₂ Evolution over Monolayer Layered Double Hydroxide under Irradiation above 600 nm

Recent Progress on Nanostructured Layered Double Hydroxides for Visible‐Light‐Induced Photoreduction of CO₂