APPLIED SURFACE SCIENCE
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2021
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IF 6.707
Xiaojing Yu,Haoran Qiu,Zhe Wang,Bin Wang,Qingnan Meng,Shaodong Sun,Yufei Tang,Kang Zhao
Aiming at comparing the charge separation efficiencies of various heterojunctions, such as p-n junction, metal–semiconductor junction, Z-scheme junction, TiO 2 -Au, TiO 2 -BiOI, TiO 2 -BiOI-Au and TiO 2 -Au-BiOI were synthesized by using n-type TiO 2 , p-type BiOI and plasmon metal Au as components for photocatalytic nitrogen fixation. The as-prepared “Z-scheme” TiO 2 -Au-BiOI photocatalyst showed the highest photocatalytic performance for N 2 photofixation with 543.53 μmol L −1 h −1 g −1 in the pure water system, which is 1.68 times higher than that of TiO 2 -BiOI-Au nanocomposite, 1.85 times higher than that of TiO 2 -BiOI and 6.69 times higher than that of TiO 2 -Au, revealing superiority of the heterojunctions of TiO 2 -Au-BiOI in kinetics among these different heterostructured photocatalysts during the photocatalytic N 2 reduction process. Moreover, the as-prepared TiO 2 -Au-BiOI exhibited considerable performance under real natural environment, showing a promising potential in future application.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2020
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IF 7.489
Zhengfeng Shen,Feifei Li,Jiangrui Lu,Zhidan Wang,Rui Li,Xiaochao Zhang,Changming Zhang,Yawen Wang,Yunfang Wang,Zhiping Lv,Jianxin Liu,Caimei Fan
Photocatalytic nitrogen fixation has been considered to be a safe, green, eco-friendly, and sustainable technology. However, photoinduced activation of inert dinitrogen is an important factor hindering the development of this technology. Herein, in-situ Fe 3+ doped flower-like BiOCl with highly active sites exposure was prepared by a solvent thermal method, which has excellent performance of N 2 photofixation. Compared with virgin BiOCl with no nitrogen fixation activity, Fe-BiOCl reached 30 μmol·L −1 ·h −1 ammonia evolution rate under simulated sunlight without any sacrificial reagent. Characterization results demonstrated that the enhancement of N 2 photofixation capacity was mainly attributed to the in-situ doped Fe 3+ in BiOCl, the doped Fe 3+ not only acts as a reaction center for N 2 activation also as an “electron transfer bridge” trapping and migrating electrons from BiOCl to N 2 molecules. Furthermore, the transformation of crystal facets from virgin BiOCl (0 0 1) to Fe-BiOCl (1 1 0) and (1 0 2) is more conducive for the exposure and accessibility of iron reactive sites. This work developed a potential strategy by in-situ introducing Fe 3+ active sites in BiOCl semiconductor substrate, which establishes a good basis for the application of semiconductor catalysts in nitrogen fixation.
研究领域:
材料科学
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环境科学
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产品关联
DOI
PubMed
高影响因子
Catalysis Science & Technology
·
2021
·Vol. 11
·期 14
·4783-4792
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IF 6.119
Yi Zhang,Shuo Gu,Xiaoyu Zhou,Kaiyue Gao,Kai Sun,Di Wu,Jingjing Xia,Xiufang Wang
Photocatalytic nitrogen fixation performance is mainly hampered by slow carrier transport and inefficient surface reaction, where surface oxygen vacancies have been proved to alleviate these limitations. However, there are a few reports on the introduction of metal vacancies into photocatalysts and the effect of metal vacancies on the N2 photofixing properties. Herein, we injected bismuth vacancies (VBi) into the surface of BiOBr nanospheres with oxygen vacancies (VO) via an ion exchange strategy to form hierarchical Bi2MoO6/BiOBr composite structures. The intentionally introduced VBi adjust the band structures of VO–BiOBr and act as charge separation centers in coordination with VO, which improves the separation efficiency of electron–hole pairs. The presence of VBi and the Bi2MoO6 phase enhances the light absorption of the composite materials. Additionally, the hierarchical nanosheet assembly structure facilitates the surface adsorption and activation of N2 on the catalyst. In particular, the optimal defect-rich Bi2MoO6/VBi+O–BiOBr exhibits the best photocatalytic ammonia production activity. After two hours, the NH3 yield was 412.18 mol L−1 without any noble metal cocatalyst and sacrificial agent, and was nearly 4 times higher than that of the original VO–BiOBr (96.08 mol L−1). This work provides a new inspiration for the design of efficient N2 immobilizing photocatalysts through synergistic metal and oxygen vacancy engineering.
研究领域:
材料科学
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环境科学
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化学工程
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Runlai Liu,Qi Chen,Jinjing Qiu,Cheng Liu,Jionghua Wu,Jimmy C. Yu,Ling Wu
The construction of metal–organic frameworks that possesses the tunable metal active sites and synergistic effect for the reactant activation is an attractive strategy for the optimization of photocatalytic performance. Herein, a series of MIL-88A(Fe 1-x Cu x ) were synthesized for photocatalytic nitrogen reduction reaction (NRR). It was characterized that the Fe 2+ and oxygen vacancies were produced in MIL-88A(Fe) due to the partly reduction of ligand fumaric acid in synthesis process. The substitution of Fe 3+ with Cu 2+ induces charge imbalance and lattice distortion, further increasing the content of Fe 2+ and oxygen vacancies. The optimal sample MIL-88A(Fe 0.95 Cu 0.05 ) (CMA-5 %) exhibits the highest nitrogen fixation performance of 68.6 μmol·g −1 ·h −1 , which is 8 times higher than that of the pristine material. It is attributable to the synergistic effect of the abundant Fe 2+ and oxygen vacancies as active sites to promote N 2 coordination and photogenerated carrier separation, resulting in the efficient conversion of activated N 2 to NH 3 . Furthermore, the in-situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy provide clear evidence of the behavior of the N 2 adsorption and activation on the catalyst. Finally, we propose a potential mechanism at molecular level regarding the relationship between the synergistic effect and the nitrogen fixation activity.
研究领域:
材料科学
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光催化
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化学工程
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产品关联
DOI
PubMed
高影响因子
RSC Advances
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2020
·Vol. 10
·期 44
·26246-26255
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IF 3.119
Zhu Ding,Shuo Wang,Xue Chang,Dan-Hong Wang,Tianhao Zhang
Photocatalytic nitrogen fixation has attracted extensive attention in recent years. Studies have shown that catalytic materials with O, N and other defects can effectively reduce the bond energy of NN triple bond when N2 is adsorbed on the defects. As an outstanding non-metallic catalyst, g-C3N4 has been widely studied in the field of photocatalytic catalysis, and the nitrogen-defected C3N4 shows promoted photocatalytic activity. Herein, nano-size MOF-74 particles (<20 nm) was dispersed on nitrogen-defected C3N4 thin film (∼4 nm) via a simple sol–gel method. The combination of Nano-MOF and defected film C3N4 could effectively improve the photocatalytic activity of nitrogen fixation through Z-scheme mechanism compared with pure defected film C3N4.
研究领域:
材料科学
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环境科学
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化学
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产品关联
DOI
PubMed
高影响因子
Molecular Catalysis
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2022
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IF 5.089
Weiwen Wang,Jianing Qu,Chaojie Li,Lexin Guo,Xianxin Fang,Guanghui Chen,Jihai Duan
Biomimetic photocatalytic nitrogen fixation is considered as a potential alternative to the Haber-Bosch method, which is an ideal pathway for nitrogen reduction. The development of efficient bionanocatalysts is a serious challenge in the current field of biomimetic nitrogen fixation. Here, we introduced a second metal in the MIL-88A/Fe mesh by metal doping to build a Mo-doped MIL-88A(Fe/Mo)/Fe mesh biomimetic system. The catalyst is a rod-like structure synthesized in situ by hydrothermal method using iron mesh as the substrate, and its rough surface is favorable for the adsorption of N 2 . The introduction of Mo provides a two-electron transfer pathway for the reaction, and the formation of the "MoFe cofactor" effectively promotes charge separation and inhibits the photoelectron-hole complexation. In addition, we kept the catalyst above the liquid surface and provided the proton source through water vapor, which solved the problem of the low solubility of N 2 in water and poor mass transfer efficiency. The results show that the biomimetic photocatalyst has good photoresponsiveness in the whole visible region, and the synergistic effect between the two metals makes the MIL-88A (Fe/Mo 0.017 )/Fe mesh exhibit better photocatalytic performance, and its nitrogen fixation efficiency reaches about 9.6 times that of the original MIL-88A/Fe mesh. This study provides a new idea for the design of photocatalytic ammonia biomimetic photocatalysts.
研究领域:
材料科学
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环境科学
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生物化学
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DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2024
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IF 5.8
Shihao Xiong,Tao Peng,Liangliang Huang,Rui wang,Beibei He,Jun Jin,Huanwen Wang,Yansheng Gong
Semiconductor photocatalytic nitrogen reduction reaction (PNRR) stands as a promising clean technique for ammonia synthesis, yet it confronts numerous challenges. In this study, Ag nanoparticle-modified Cu-doped Bi 2 WO 6 (ACB) porous composite materials with varying mass percentages were successfully synthesized using a solvothermal reduction approach. The incorporation of transition metal Cu effectively modulates the energy band position of Bi 2 WO 6 . Furthermore, the introduction of Ag nanoparticles significantly suppresses the recombination of photogenerated carriers. Without adding sacrificial agent, the photocatalytic nitrogen fixation yield of ACB reaches an impressive 184.93 μmol·g −1 ·h −1 , which is 5.44 times higher than that of pristine Bi 2 WO 6 . A comprehensive analysis of the experimental results reveals that the combined effect of Cu doping and Ag nanoparticle loading endows ACB with an increased exposure of active sites, thereby significantly enhancing its photocatalytic nitrogen fixation performance. This research offers a promising approach for the design of metal nanoparticle-supported catalysts for PNRR, holding significant implications for the advancement of other material systems.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
Surfaces and Interfaces
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2024
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IF 5.7
Qian Cheng,Xiaohan Liu,Chuhan Huang,Hongman Sun,Fazle Subhan,Xinyi Zhou,Yuankai Liu,JiaHui Yang,Qi Li,Youhe Wang,Zifeng Yan
Recently, there has been a growing interest in the fundamental understanding of the mechanism of how MIL-101(Fe)/g-C 3 N 4 heterojunctions facilitate the occurrence of photocatalytic nitrogen fixation reactions, especially the electron transfer mechanism has attained increasing attention in photocatalysis. Herein, we implemented a "triple win scenario" strategy to fabricate the S-scheme MIL-101(Fe)/g-C 3 N 4 heterojunction through a straightforward solvothermal process. The MC-6 heterojunction minimizes the recombination of photogenerated carriers, enhances light utilization efficiency, and activates the N≡N bond, thus boosting photocatalytic nitrogen fixation efficiency. The transition metal iron activates the N≡N bond, while S-scheme heterojunctions reduce the photogenerated carrier recombination. In addition, the decrease in band gap (E g ) leads to an increase in visible light utilization efficiency. ISIXPS proved the mechanism of interelectron transfer of MIL-101(Fe)/g-C 3 N 4 heterojunction under illumination. Upon the creation of the heterojunction, electrons migrate from g-C 3 N 4 to MIL-101(Fe), establishing an inherent electric field due to the disparate Fermi levels between the two materials. The electrons (e - ) on the g-C 3 N 4 CB with a more negative reduction potential and the holes ( h + ) on the MIL-101(Fe) VB are retained, which increased the redox capacity to a great extent required for the reduction of N 2 to NH 3 . The ammonia production efficiency of MC-6 photocatalyst was 160 µmol g cat -1 h -1 , representing an 8-fold and 2.8-fold improvement over pristine g-C 3 N 4 (20 µmol g cat -1 h -1 ) and MIL-101(Fe) (57 µmol g cat -1 h -1 ), respectively.
研究领域:
材料科学
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环境科学
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化学
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
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2021
·
IF 8.271
Xue Chen,Ming-Yu Qi,Yue-Hua Li,Zi-Rong Tang,Yi-Jun Xu
The fabrication of efficient catalysts to reduce nitrogen (N 2 ) to ammonia (NH 3 ) is a significant challenge for artificial N 2 fixation under mild conditions. In this work, we demonstrated that the simultaneous introduction of oxygen vacancies (OVs) and Mo dopants into Bi 5 O 7 Br nanosheets can significantly increase the activity for photocatalytic N 2 fixation. The 1 mol% Mo-doped Bi 5 O 7 Br nanosheets exhibited an optimal NH 3 generation rate of 122.9 μmol g −1 h −1 and durable stability, which is attributed to their optimized conduction band position, suitable absorption edge, large number of light-switchable OVs, and improved charge carrier separation. This work provides a promising approach to design photocatalysts with light-switchable OVs for N 2 reduction to NH 3 under mild conditions, highlighting the wide application scope of nanostructured BiOBr-based photocatalysts as effective N 2 fixation systems.
研究领域:
材料科学
·
催化
·
光化学
✓ 已验证
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2023
·
IF 8.4
Sitong Liu,Guangmin Ren,Xiangchao Meng
A BrO3–-modified Bi2O3/Bi(OH)3 heterojunction photocatalyst was in situ fabricated by a facile one-pot method and applied in photocatalytic nitrogen fixation. In comparison with Bi(OH)3, the Bi2O3/Bi(OH)3 heterojunction has a larger specific surface area from the nanoflower-like morphology and an extended visible light absorption range. Of special importance, the proper band gap match between Bi(OH)3 and Bi2O3, the multiple charge transfer channels via the BrO3– bridge, and the oriented electron migration in the type-II heterojunction mechanism make a stronger charge separation efficiency. Therefore, the BiO/BiHO-3 sample presented the highest photocatalytic nitrogen reduction performance with an ammonia production rate of 45.28 μmol g–1 h–1, which was 10 times higher than that of Bi(OH)3. Photogenerated cavities are consumed during H2O oxidation to produce O2 and H2O2. However, the O2 production was small, and the H2O2 yield was about 78.5 μmol g–1 h–1. For CO2 reduction, the CO production rate was 52.86 μmol g–1 h–1, which was 1.6 and 1.9 times those of Bi(OH)3 and Bi2O3. This work provides useful guidance for the design and synthesis of efficient catalysts for photocatalytic N2 fixation.
研究领域:
材料科学
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环境科学
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化学
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产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
·
IF 19.503
Xiufan Liu,Yani Luo,Cancan Ling,Yanbiao Shi,Guangming Zhan,Hao Li,Huayu Gu,Kai Wei,Furong Guo,Zhihui Ai,Lizhi Zhang
Herein, we demonstrate that the rare-earth La single catalyst with multi-shell characteristic is an excellent choice for this purpose. By merit of its unsaturated orbitals of La, the single La atom strongly bonds with the two-coordinated lattice oxygen on the oxygen-deficient MoO 3−x to form O 2c -La-O 2c coordination. This robust metal-support interaction frees single atoms from detachment or aggregation, and prevents catalyst from deactivation. Meanwhile, the occupied 5d orbitals of La back-donate electrons to the 2π* molecular orbitals of adsorbed N 2 that substantially activate the inert N N bond towards successive hydrogenation. And single La atom could optimize the electron property of the MoO 3−x support to promote photocatalytic nitrogen fixation. Without any sacrificial agents, this single atom La catalyst with a well-designed coordination structure delivers an impressive NH 3 production rate of 209.0 μmol h 1 g 1 under visible light, outperforming most reported single atom photocatalysts.
研究领域:
材料科学
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催化化学
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环境科学
✓ 已验证
DOI
高影响因子
JOURNAL OF SOLID STATE CHEMISTRY
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2020
·
IF 2.726
Guoqiang Li,Feifei Li,Jianxin Liu,Caimei Fan
The nitrogen activation is the Achilles’ heel of photocatalytic nitrogen fixation . Herein, metal-organic frameworks (MOFs), for first time, are proposed to solve the above bottleneck. A series of Fe-Based MOFs (MIL-101(Fe), MIL-100(Fe), MIL-88(Fe)) demonstrated excellent photocatalytic nitrogen fixation activity. To gain insight into the reaction mechanism, MIL-101(Cr) and MIL-101(Fe), with same molecular structure except the central metal ions , selected for system comparison. Photocatalytic nitrogen fixation activity of MIL-101(Fe) and MIL-101(Cr) are 50.355 μmol L −1 h −1 and inactive, respectively. This suggested that the nitrogen fixation activity originated from the Fe catalytic center. The results of in situ FTIR and quantum computation verifies Fe catalytic center have a higher electron density, a lower reaction activation energy and more generation of N–H bond than those of Cr catalytic center. In view of the analogous outer electron configuration of Cr and Fe, it was suspect that two extra d-orbitals electronics of Fe element are the basic reason of the excellent photocatalytic nitrogen fixation activity. This work provides a new application of MOFs in photocatalytic nitrogen fixation field and emphasizes the vital of d-orbitals electronics during the nitrogen activation process.
研究领域:
材料科学
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催化化学
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）