Toward visible-light-assisted photocatalytic nitrogen fixation: A titanium metal organic framework with functionalized ligands

Huang, Hao; Wang, Xusheng; Philo, Davin; Ichihara, Fumihiko; Song, Hui; Li, Yunxiang; Li, Dan; Qiu, Teng; Wang, Shengyao; Ye, Jinhua

doi:10.1016/j.apcatb.2020.118686

Cited by 197 publications

(146 citation statements)

References 39 publications

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“…Recently, this strategy has been used widely in different applications. [ 124,125 ] Huang et al. synthesized a series of OH‐MIL‐125(Ti), NH 2 ‐MIL‐125(Ti), and CH 3 ‐MIL‐125(Ti) as photocatalysts for NRR by using SALE approach and one‐pot synthesis (Figure 6d).…”

Section: Defects In Mofsmentioning

confidence: 99%

The Role of Defects in Metal–Organic Frameworks for Nitrogen Reduction Reaction: When Defects Switch to Features

Khalil

Xue

Liu

et al. 2021

Adv Funct Materials

119

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The electrochemical nitrogen reduction reaction (NRR), a contributor for producing ammonia under mild conditions sustainably, has recently attracted global research attention. Thus far, the design of highly efficient electrocatalysts to enhance NRR efficiency is a specific focus of the research. Among them, defect engineering of electrocatalysts is considered a significant way to improve electrocatalytic efficiency by regulating the electronic state and providing more active sites that can give electrocatalysts better physicochemical properties. Recently, metal–organic frameworks (MOFs), along with their derivatives, have captured immense interest in electrocatalytic reactions owing to not only their large surface area and high porosity but also the ability to create rich defects in their structures. Hence, they can provide plenty of exposed active sites for electron transfer, NN cleavage, and N2 adsorption to enhance NRR performance. Herein, the concept, the in situ characterizations techniques for defects, and the most common ways to create defects into MOFs have been summarized. Furthermore, the recent advances of MOF‐based electrocatalysts towards NRR have been recapitulated. Ultimately, the major challenges and outlook of defects in MOFs for NRR are proposed. This paper is anticipated to provide critical guidelines for optimizing NRR electrocatalysts.

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Section: Defects In Mofsmentioning

confidence: 99%

The Role of Defects in Metal–Organic Frameworks for Nitrogen Reduction Reaction: When Defects Switch to Features

Khalil

Xue

Liu

et al. 2021

Adv Funct Materials

119

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“…[ 147 ] In 2020, Ye and coworkers found NH 2 ‐MIL‐125(Ti) with the integration of Ti sites and amine‐functionalized linkers exhibited the photoreduction ability of N 2 to NH 3 with a rate of 12.3 μmol g −1 h −1 under visible light illumination. [ 148 ] Fan's group synthesized a series of Fe‐based MOFs (MIL‐101(Fe), MIL‐100(Fe), MIL‐88(Fe)) with excellent photocatalytic NRR activity, and found that the active sites for nitrogen fixation are Fe catalytic centers. [ 149 ] Shi and coworkers reported a new viologen‐based radical‐containing MOFs (Gd‐IHEP‐7), which could be heated in air to form Gd‐IHEP‐8, [ 150 ] and the Gd‐IHEP‐7 and Gd‐IHEP‐8 showed NH 3 yield of 128 and 220 μmol g −1 h −1 without sacrificial agent, respectively.…”

Section: Photocatalysts For Nitrogen‐fixation Reactionmentioning

confidence: 99%

Fundamentals and Recent Progress of Photocatalytic Nitrogen‐Fixation Reaction over Semiconductors

2020

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As a green energy carrier, a potential fuel and an essential chemical for the manufacturing of fertilizers, plastics, and explosives, ammonia (NH3) is currently produced by Haber−Bosch process. However, the process converting nitrogen (N2) into NH3 under strict conditions consumes substantial energy and releases enormous greenhouse gases. In the context of the global energy crisis and increasing greenhouse effect, it is urgent to explore mild, green, sustainable, and economic nitrogen‐fixation strategies. Very recently, photocatalytic nitrogen‐fixation reactions, including nitrogen reduction reaction (NRR) and nitrogen oxidation reaction (NOR), have aroused widespread attention due to its environmental friendliness and cost‐effectiveness. To achieve high photocatalytic performance and selectivity, it is necessary to design photocatalyst and its photoreaction system reasonably to optimize the light absorption, charge separation, mass transport, adsorption, and activation of N2 as well as proton/electron transfer. This review gives an overview of fundamentals, performance evaluation, and recent progress of the photocatalytic nitrogen‐fixation reactions. The photocatalysts and their design strategies are classified, and several suggestions are given for the analysis of the existing photocatalytic nitrogen‐fixation systems. Finally, a short perspective on the existing challenges and future opportunities are outlined for providing insights into the development of high‐efficiency photocatalytic systems for artificial N2 fixation.

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Section: Inorganic Pollutants Remediationmentioning

confidence: 99%

“…With this in mind, our group first reported a series of photoresponsive titanium‐based MOFs for nitrogen fixation under visible light irradiation. [ 24 ] Three visible light active Ti‐MOFs, named CH 3 ‐MIL‐125(Ti), OH‐MIL‐125(Ti), and NH 2 ‐MIL‐125(Ti), were synthesized by one‐pot synthesis or solvent‐assistant ligand exchange methods ( Figure ). Compared with the pristine MIL‐125(Ti), all of those three ligand‐modified MOFs exhibited extended light absorption range, following the order of CH 3 ‐MIL‐125(Ti) < OH‐MIL‐125(Ti) < NH 2 ‐MIL‐125(Ti).…”

Section: Photocatalytic Applicationsmentioning

confidence: 99%

“…For instance, a recent study by our group found that amino‐modified NH 2 ‐MIL‐125 could photoreduce N 2 into NH 3 under visible light irradiation in pure water. [ 24 ] As related studies have been growing rapidly, a comprehensive understanding of the chemistry of titanium‐based MOFs is highly desired. Pioneers have given the summary on the synthetic approaches involving direct synthesis and post‐metathesis.…”

Section: Introductionmentioning

confidence: 99%

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Titanium‐Based MOF Materials: From Crystal Engineering to Photocatalysis

et al. 2020

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Titanium (Ti)‐based metal–organic frameworks (MOFs) have attracted intensive attention due to the low toxicity, high earth's crust abundance, and unique photocatalytic properties of Ti elements. Great efforts have been devoted to the synthesis of novel architectures and their potential applications involving photocatalysis. However, Ti‐MOFs are still very scarce owing to their challenges in controlling the Ti chemistry in the reaction system. Until now, some significant results have been achieved, which may shed new insight into the future investigation of Ti‐MOFs. Herein, some representative researches in Ti‐MOFs are summarized and reviewed from the following four aspects: first, various synthetic strategies for preparing Ti‐MOFs are introduced; second, diverse structures containing multi‐connected ligands are presented in detail; third, the potential photocatalytic applications of Ti‐based MOFs involving H2 production, CO2 reduction, H2O2 production, N2 fixation, remediation of organic and inorganic pollutants, as well as organic transformation reaction and photocatalytic sensors are discussed; finally, perspectives on current challenges and emerging opportunities in this research field are discussed. Through summarizing this specific type of MOF, this review is expected to stimulate researchers’ interest for in‐depth investigation of novel structures synthesis, as well as new applications and concepts in these intriguing fields.

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Toward visible-light-assisted photocatalytic nitrogen fixation: A titanium metal organic framework with functionalized ligands

Cited by 197 publications

References 39 publications

The Role of Defects in Metal–Organic Frameworks for Nitrogen Reduction Reaction: When Defects Switch to Features

The Role of Defects in Metal–Organic Frameworks for Nitrogen Reduction Reaction: When Defects Switch to Features

Fundamentals and Recent Progress of Photocatalytic Nitrogen‐Fixation Reaction over Semiconductors

Titanium‐Based MOF Materials: From Crystal Engineering to Photocatalysis

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