Nitrogenase-inspired bimetallic metal organic frameworks for visible-light-driven nitrogen fixation

An, Ke; Ren, Hanjie; Yang, Dong; Zhao, Zhanfeng; Gao, Y.C.; Chen, Yao; Tan, Jiangdan; Wang, Wenjing; Jiang, Zhongyi

doi:10.1016/j.apcatb.2021.120167

Cited by 67 publications

(58 citation statements)

References 62 publications

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“…53 Then, the electron is further excited by the second photon and transfers to a higher excited state that can provide enough energy for the next step. 8 Furthermore, through the continuous energy band, the electron transfers to the bimetallic Ce-Hf cluster, which is consistent with the reported result in the literature. 53,54 In order to verify the electron transfer path in the bimetallic Ce-Hf sites, the flat band potentials of the Ce-O or Hf-O cluster in the metallic phase materials were tested by the Mott-Schottky curves.…”

Section: Photocatalytic Mechanismsupporting

confidence: 91%

“…Recently, benefited from the modular property, uniform pore structure and well crystal texture, metal organic frame materials (MOFs) have become an ideal platform for the rational design of high-efficiency N 2 fixation photocatalysts. [7][8][9][10] For example, Huang et al achieved a photocatalytic nitrogen fixation efficiency at a rate of 12.3 μmol g −1 h −1 by amino-functionalizing the organic ligand of MIL-125 (Ti). 11 Introducing the rare-earth Ce element into the metal cluster nodes of MOF-76, Zhang et al simulated the biogenic π backdonation mechanism to obtain a nitrogen fixation rate of 34 μmol g −1 h −1 at room temperature.…”

Section: Introductionmentioning

confidence: 99%

“…13 In addition, inspired by the multi-metal cluster structure of biological nitrogenases, we designed a kind of UiO-66 photocatalyst composed of bimetallic Zr-Hf nodes, which exhibited the improved photocatalytic N 2 fixation performance in the previous study. 8 However, the role of bimetal nodes is still obscure in the electron transfer and utilization process, which needs to be studied intensively.…”

Section: Introductionmentioning

confidence: 99%

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Modular assembly of electron transfer pathways in bimetallic MOFs for photocatalytic ammonia synthesis

Tan

Yang

et al. 2022

Catal. Sci. Technol.

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Section: Photocatalytic Mechanismsupporting

confidence: 91%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Modular assembly of electron transfer pathways in bimetallic MOFs for photocatalytic ammonia synthesis

Tan

Yang

et al. 2022

Catal. Sci. Technol.

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“…2 Because of the very high bond energy of NN, the HB process not only brings about potential danger but also consumes fossil energy. 3 It is obvious that the HB process is an energy-and costexpensive process as well as a harmful process to the environment. Hence, it is necessary to develop a low cost and energy-saving method to convert N 2 to NH 3 .…”

Section: ■ Introductionmentioning

confidence: 99%

“…In industry, ammonia is mainly produced via Haber–Bosch (HB) process, which uses ruthenium or iron-based catalysts at a high temperature and pressure . Because of the very high bond energy of NN, the HB process not only brings about potential danger but also consumes fossil energy . It is obvious that the HB process is an energy- and cost-expensive process as well as a harmful process to the environment.…”

Section: Introductionmentioning

confidence: 99%

Bismuth Semimetal-Boosted Electron Transfer, Nitrogen Adsorption, and Nitrogen Photoreduction Activity of Bi/g-C₃N₄ Nanosheets

Chen

Liang

et al. 2021

Energy Fuels

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Nitrogen photoreduction is a promising ammonia production technology since it can be carried out at the atmospheric pressure by merely utilizing the abundant solar energy. However, the low conversion efficiency is still a big challenge for practical applications. In this work, Bi-decorated g-C 3 N 4 nanosheets are successfully prepared by an in situ solvothermal method. The ultraviolet−visible diffuse reflection spectrum shows that Bi decoration conspicuously enhances the visible light absorption because of the surface plasmon resonance effect of the Bi semimetal. Moreover, the photoluminescence spectrum demonstrates that Bi decoration greatly improves the charge separation efficiency because the high work function of Bi (4.5 eV) favors electron transfer from the conduction band of g-C 3 N 4 to the Bi surface. Meanwhile, nitrogen sorption isotherms show that Bi decoration obviously increases the Brunauer−Emmett−Teller surface area (4.3 m 2 g −1 for g-C 3 N 4 vs 7.7−8.4 m 2 g −1 for Bi/g-C 3 N 4 ), which is beneficial for N 2 adsorption. Additionally, the density functional theory calculation shows that the adsorption energy (E ad ) of N 2 on Bi/g-C 3 N 4 (−2.3 eV) is 6.2 times higher than that on g-C 3 N 4 (−0.3 eV), which indicates that N 2 is easier to adsorb on Bi/g-C 3 N 4 thermodynamically. It is assumed that the decorated Bi can also provide new active sites that significantly improve the adsorption and activation of N 2 . Therefore, Bi/g-C 3 N 4 exhibits a high nitrogen photoreduction activity under visible light irradiation (λ > 420 nm): the ammonia yield over 30-Bi/g-C 3 N 4 (3075 μmol L −1 g −1 ) is 1.8 times higher than that over g-C 3 N 4 (1076 μmol L −1 g −1 ) and the ammonia production rate over 30-Bi/g-C 3 N 4 (1025 μmol L −1 g −1 h −1 ) is 1.8 times higher than that over g-C 3 N 4 (359 μmol L −1 g −1 h −1 ). The improved activity is mainly attributed to the Bi decoration on the g-C 3 N 4 surface, which improves the adsorption and activation of N 2 , the electron−hole separation efficiency, and the light-harvesting ability. This work demonstrates that similar to precious metals, Bi semimetal can also greatly improve the nitrogen photoreduction activity. Most importantly, Bi semimetal is more abundant and cheaper than precious metals, and it could be more promising for practical applications.

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A Review of MOFs and Their Composites‐Based Photocatalysts: Synthesis and Applications

Qian

Zhang

Pang

2021

Adv Funct Materials

280

157

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Photocatalysis is considered to be a green and environment‐friendly technology since it can convert solar energy into other types of chemical energies. Over the past several years, metal‐organic frameworks (MOFs)‐based photocatalysts have received remarkable research interest due to their unique morphology, high photocatalytic performance, good chemical stability, easy synthesis, and low cost. In this review, the synthetic strategies of developing MOFs‐based photocatalysts are first introduced. Second, the recent progress in the fabrication of various types of MOFs composites photocatalysts is summarized. Third, the different applications including hydrogen evolution reaction, oxygen evolution reaction, overall water splitting, nitrogen reduction reaction, carbon dioxide reduction reaction as well as photodegradation of organic pollutants of MOFs‐based photocatalysts are summed up. Finally, the challenges and some suggestions for the future development of MOFs‐ and their composites‐based photocatalysts are also highlighted. It is expected that this report will help researchers to systematically devise and develop highly efficient photocatalysts based on MOFs and their composites.

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Nitrogenase-inspired bimetallic metal organic frameworks for visible-light-driven nitrogen fixation

Cited by 67 publications

References 62 publications

Modular assembly of electron transfer pathways in bimetallic MOFs for photocatalytic ammonia synthesis

Modular assembly of electron transfer pathways in bimetallic MOFs for photocatalytic ammonia synthesis

Bismuth Semimetal-Boosted Electron Transfer, Nitrogen Adsorption, and Nitrogen Photoreduction Activity of Bi/g-C₃N₄ Nanosheets

A Review of MOFs and Their Composites‐Based Photocatalysts: Synthesis and Applications

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Nitrogenase-inspired bimetallic metal organic frameworks for visible-light-driven nitrogen fixation

Cited by 67 publications

References 62 publications

Modular assembly of electron transfer pathways in bimetallic MOFs for photocatalytic ammonia synthesis

Modular assembly of electron transfer pathways in bimetallic MOFs for photocatalytic ammonia synthesis

Bismuth Semimetal-Boosted Electron Transfer, Nitrogen Adsorption, and Nitrogen Photoreduction Activity of Bi/g-C3N4 Nanosheets

A Review of MOFs and Their Composites‐Based Photocatalysts: Synthesis and Applications

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Bismuth Semimetal-Boosted Electron Transfer, Nitrogen Adsorption, and Nitrogen Photoreduction Activity of Bi/g-C₃N₄ Nanosheets