Catalysts
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2020
·Vol. 10
·期 9
·1027
·
IF 3.52
Binxiang Cai,Huazhang Liu,Wenfeng Han
Fe2O3-based catalysts were prepared by solution combustion synthesis (SCS) with metal nitrates (Fe, K, Al, Ca) as the precursors and glycine as the fuel. The activities of catalysts were evaluated in terms of ammonia synthesis reaction rate in a fixed bed reactor similar to the industrial reactors. The results indicate that the precursor of catalyst prepared by SCS is Fe2O3which facilitates the high dispersion of promoters to provide high activity. The catalysts exhibit higher activity for ammonia synthesis than that of traditional catalysts, and the reaction rate reaches 138.5 mmol g−1h−1. Fe2O3prepared by SCS could be favorable precursor for ammonia synthesis catalyst. The present study provides a pathway to prepare catalyst for ammonia synthesis.Keywords:ammonia synthesis;catalyst;Fe2O3;solution combustion synthesis
研究领域:
化学工程
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催化科学
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产品关联
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2023
·
IF 9.2
Dekun Shi,Zhaojun Shi,Lixin Zhang,Yaan Cao
This study presents a novel fluorine and iodine co-doped Bi 2 MoO 6 (Bi 2 MoO 6 –F–I) photocatalyst prepared using a solvothermal method . The photocatalytic performance of Bi 2 MoO 6 –F–I in N 2 photocatalytic reduction to NH 3 is considerably enhanced compared to that of pristine Bi 2 MoO 6 . The experimental findings and theoretical calculations reveal that F − substitute lattice O 2− in Bi 2 MoO 6 , creating a -Mo-F-Mo- configuration, while I − modifies the surface, forming -Bi-I species in Bi 2 MoO 6 –F–I, which serve as high-adsorption centres and active surface sites, facilitating N 2 and H 2 O molecule adsorption and activation on the surface. The synergistic effect of F − doping and -Bi-I surface species optimizes the band structure of Bi 2 MoO 6 –F–I, aligning more effectively with the redox potential of N 2 photoreduction, which consequently promotes photogenerated carrier separation and redox capability. The remarkable improvement in the photocatalytic performance of Bi 2 MoO 6 –F–I in N 2 photoreduction to NH 3 lays foundation for designing and fabricating high-performance Bi 2 MoO 6 -based photocatalysts.
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
Chemistry-An Asian Journal
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2020
·Vol. 15
·期 8
·1272-1276
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IF 4.056
Yueming Cao,Peipei Li,Tengteng Wu,Meiling Liu,Youyu Zhang
Graphical HKUST-1 (Cu−BTC, BTC=benzene-1,3,5 tricarboxylate) was selected as an electrocatalyst for the reaction of conversion N 2 to NH 3 under ambient conditions. At −0.75 V vs. reversible hydrogen electrode, it achieves excellent performance with high NH 3 yield (46.63 μg h −1 mg −1 cat. or 4.66 μg h −1 cm −2 ) and Faraday efficiency (2.45%). Electrolytic ammonia synthesis from nitrogen at ambient conditions is appearing as a promising alternative to the Haber-Bosch process which is consuming high energy and emitting CO 2 . Here, a typical MOF material, HKUST-1 (Cu−BTC, BTC=benzene-1,3,5-tricarboxylate), was selected as an electrocatalyst for the reaction of converting N 2 to NH 3 under ambient conditions. At −0.75 V vs. reversible hydrogen electrode, it achieves excellent catalytic performance in the electrochemical synthesis of ammonia with high NH 3 yield (46.63 μg h −1 mg −1 cat. or 4.66 μg h −1 cm −2 ) and good Faraday efficiency (2.45%). It is indicated that the good performance of the HKUST-1 catalyst may originate from the formation of Cu(I). In addition, the catalyst also has good selectivity for N 2 to NH 3 .
研究领域:
材料科学
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电化学
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催化反应
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
·
IF 9.965
Xun He,Long Hu,Lisi Xie,Zerong Li,Jie Chen,Xiuhong Li,Jun Li,Longcheng Zhang,Xiaodong Fang,Dongdong Zheng,Shengjun Sun,Jing Zhang,Abdulmohsen Ali Alshehri,Yongsong Luo,Qian Liu,Yan Wang,Xuping Sun
Nitrite (NO 2 − ), as a N -containing pollutant, widely exists in aqueous solution, causing a series of environmental and health problems. Electrocatalytic NO 2 − reduction is a promising and sustainable strategy to remove NO 2 − , meanwhile, producing high value-added ammonia (NH 3 ). But the NO 2 − reduction reaction (NO 2 − RR) involves complex 6-electron transfer process that requires high-efficiency electrocatalysts to accomplish NO 2 − -to-NH 3 conversion. Herein, we report NiS 2 nanoparticles decorated TiO 2 nanoribbon array on titanium mesh (NiS 2 @TiO 2 /TM) as a fantastic NO 2 − RR electrocatalyst for ambient NH 3 synthesis. When tested in NO 2 − -containing solution, NiS 2 @TiO 2 /TM achieves a satisfactory NH 3 yield of 591.9 µmol h −1 cm −2 and a high Faradaic efficiency of 92.1 %. Besides, it shows remarkable stability during 12-h electrolysis test.
研究领域:
环境科学
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材料科学
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电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
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2022
·Vol. 28
·期 33
·e202200779
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IF 5.02
Wei Xiong,Min Zhou,Xiaoyan Huang,Weijie Yang,Da Zhang,Yaokang Lv,Hao Li
Graphical A novel interlaced mesoporous NiO NSs@CF electrochemical catalyst was prepared using a direct in situ vertical growth method, in which NiO formed mesoporous nanosheets with a pore size of 15 nm and a thickness of ∼30 nm. This binder-free electrode exhibited a superior NH 3 yield of 71.3 μg h −1 mg −1 cat. and a FE of 17.9 % at −0.5 V vs. RHE. Metal oxide nanomaterials directly grown on conductive substrates are optimal electrode materials because their structures allow for rapid ion and electron transport and thereby reduce internal resistance in the electrode. The development of such binder-free, self-supporting electrodes is of great significance for applications in electrocatalysis. In this work, a simple hydrothermal in situ self-assembly reaction and annealing process was developed to prepare three kinds of nickel oxide @ carbon felt (NiO@CF) nanocomposites with different morphologies. The influence of different precipitators (strong or weak bases) on the morphology of the resulting nano-sized nickel oxide nanocomposites was investigated. The microstructures of the NiO@CF samples were characterized with field emission scanning electron microscopy (FESEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS). When ammonia was used as the precipitator, NiO grew vertically on the surface of the carbon felt and formed a mesoporous nanosheet-like structure (NiO NSs@CF). As an electrocatalytic nitrogen reduction reaction ( e -NRR) electrode, the NiO NSs@CF sample showed an excellent NH 3 yield (71.3 μg h −1 mg −1 cat. ) and Faradaic efficiency (17.9 % at −0.5 V vs. RHE) in 0.1 M Na 2 SO 4 . The good performance was attributed to the vertical interleaved mesoporous sheet-like structure (with the pore size of 15 nm and the thickness of ∼30 nm) and the relatively high concentration of oxygen vacancies. First-principles calculations with strong on-site Coulomb interactions demonstrated that the presence of oxygen vacancy on NiO sample leads to a significantly stronger N binding over the surface, benefiting for the nitrogen gas adsorption and reduction. The e -NRR performance of this binder-free, flexible electrode material is superior to that of other reported nickel-based nanomaterials. This study highlights the potential of such binder-free carbon felt electrodes for use in e -NRR that could meet the needs of industrial production.
研究领域:
材料科学
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电化学
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
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2020
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IF 8.758
Xue Zhao,Ziqiong Yang,Artem V. Kuklin,Glib V. Baryshnikov,Hans Ågren,Xiaohai Zhou,Haibo Zhang
Currently, the development of stable electrochemical nitrogen reduction reaction (ENRR) catalysts with high N2 conversion activity and low cost to instead of the traditional Haber-Bosch ammonia production process of high-energy consumption remains a great challenge for researchers. Here, we have immobilized reductive closo-[B12H11]− boron clusters on a carbon nanotubes (CNT) surface and have successfully prepared a novel Au-CNT catalyst with extraordinary ENRR activity after adding HAuCl4 to the CNT-[B12H11]− precursor. The excellent properties of ammonia yield (57.7 μg h–1 cm–2) and Faradaic efficiency (11.97%) make it possible to achieve using this Au-CNT catalyst in large-scale industrial production of ammonia. Furthermore, its outstanding cyclic stability and long-term tolerability performance make it one of the most cost-effective catalysts to date. Here, by means of density functional theory we disclose the associative mechanism of N2-to-NH3 conversion on the Au(111) surface, providing visual theoretical support for the experimental results.
研究领域:
材料科学
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化学工程
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理论化学
✓ 已验证
DOI
高影响因子
JOURNAL OF RARE EARTHS
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2020
·
IF 3.104
Wei Li,Shuang Wang,Jinping Li
A series of BaCeO 3 modified with different rare earth elements (La, Y, Pr) were synthesized by co-precipitation and calcination and the effect of rare earth elements for catalytic ammonia synthesis under mild conditions was studied. The ammonia synthesis performance tests show that 2.5% Ru/BaCe 0.9 La 0.1 O 3– δ catalyst (All the percentages of Ru in this article are in mass fraction) exhibits the highest ammonia synthesis rate (34 mmol/(g·h)) at 3 MPa, 450 °C, and no sign of deactivation after 100 h of reaction. H 2 -TPR and XPS analyses indicate that the introduction of La increases the amount of oxygen vacancies of the catalyst, which is beneficial to increasing the electron density of Ru surface. HRTEM analysis shows that the Ru particle size is reduced greatly after La is introduced, which facilitates the catalyst generating more B 5 -type sites (active sites of Ru species for N N dissociation). CO 2 -TPD analysis indicates that BaCe 0.9 La 0.1 O 3– δ has stronger basicity , which promotes electrons transfer from support to Ru. This work provides an effective method for design and synthesis of Ru-based multi-element composite perovskite oxide catalysts.
研究领域:
催化化学
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材料科学
✓ 已验证
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2025
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IF 3.9
Cuilian Sun,Huhu Yin,Xiujing Xing,Yaokang Lv,Wei Xiong,Hao Li
In recent years, a variety of catalysts have been applied to electrocatalytic nitrogen reduction (NRR). Previous research has shown that in bimetallic catalysis the synergistic effect between the bimetals results in catalytic properties superior to those of monometallic catalysts. In this work, bimetallic oxide MnMoO4 nanomaterials with different particle sizes were prepared by a solvothermal method, and the effects of different ratios of the solvents (water/ethylene glycol) on the particle sizes of MnMoO4 and their influence on the NRR performance were systematically investigated. The results showed that as the proportion of ethylene glycol solvent increased, scanning electron microscopy (SEM) characterization showed a transformation of morphology from micrometer-scale rods to nanoscale particles, and the smallest MnMoO4 particle size was obtained at a water/ethylene glycol ratio of 0:1. Under this condition, the formed MnMoO4 exhibited excellent NRR properties at −0.40 V vs RHE with an NH3 yield as high as 21.89 μg h–1 mgcat–1 and a Faraday efficiency (FE) of 15.12%, with the best stability among all catalysts synthesized in this work. This may be attributed to the increased viscosity of the ethylene glycol environment, leading to a deceleration of the precursor reactions. This leads to the production of materials with smaller particle sizes, exposing more active sites and improving catalytic performance. In addition, we explored the effect of other solvents (n-butanol and glycerol) on the morphology of the materials. This work indicates that changing the solvent to regulate the morphology and size of the bimetallic oxide MnMoO4 can improve the catalytic efficiency of the catalyst, providing a promising electrocatalyst for nitrogen reduction reactions.
研究领域:
材料科学
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催化化学
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能源化学
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产品关联
DOI
高影响因子
ACS Applied Energy Materials
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2021
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IF 6.024
Peixin Liu,Peng Jing,Xuan Xu,Baocang Liu,Jun Zhang
The electrochemical synthesis of ammonia from N2 under mild conditions is a promising alternative to the energy-consuming Haber–Bosch process. Metal–organic frameworks (MOFs) are promising electrocatalysts for the N2 reduction reaction, but most of them are active for the undesirable and competitive hydrogen evolution reaction. Herein, we developed a facile strategy to grow a Ce-MOF on copper mesh substrate. The Ce-MOF with a self-supporting structure could be directly used as an electrode for the N2 reduction reaction, demonstrating highly efficient electrocatalytic performance with an NH3 yield of 14.83 μg h–1 cm–2 and a Faradaic efficiency of 10.81% at −0.2 V versus a reversible hydrogen electrode. Structural characterizations of Ce-MOF after electrocatalysis revealed that Ce-MOF as precatalyst underwent structural reconstruction at negative potential, forming catalytically active CeO2 with oxygen vacancies embedded in the amorphous Ce-MOF. In addition, the self-supporting structure formed by in situ growth of Ce-MOF on porous and conductive cooper mesh endowed the electrocatalyst with enhanced stability, conductivity, and mass transport. This work demonstrated the structural transformation of Ce-MOF during the electrocatalytic process and provided new insight for the rational design of MOF-based electrocatalysts.
研究领域:
材料科学
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电化学
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催化反应
✓ 已验证
产品关联
DOI
高影响因子
DALTON TRANSACTIONS
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2023
·Vol. 52
·期 45
·16670-16679
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IF 4
Huhu Yin,Xiujing Xing,Wei Zhang,Jin Li,Wei Xiong,Hao Li
Electrocatalytic nitrogen reduction (NRR) for artificial ammonia synthesis under ambient conditions is considered a promising alternative to the traditional Haber–Bosch process. However, it still faces multiple challenges such as the difficulty of N2 adsorption and activation and limited Faraday efficiency. In this work, a bimetallic oxide MnMoO4 was prepared by a hydrothermal method and low temperature calcination. The influence of the sintering temperature on the microstructure (crystallinity and oxygen vacancies) of the oxide and its NRR properties were systematically explored. The results showed that MnMoO4 sintered at 500 °C had the highest concentration of OVs and showed excellent NRR performance, with the highest NH3 yield (up to 12.28 μg h−1 mgcat−1), high Faraday efficiency (23.04% at −0.30 V vs. RHE), and good stability at −0.40 V vs. RHE, and the catalytic performance was about two times higher than that of Mn2O3 and MoO3. It is also superior to other bimetallic oxide NRR electrocatalysts reported in some cases. In addition, we also explored the ratio between Mn and Mo metals, and the catalytic effect was the best when Mn : Mo = 1 : 1. Due to the synergistic effect between Mn and Mo metals and the large number of OVs present internally, the catalytic activity for the NRR was largely improved. This study suggests that the bimetallic oxide MnMoO4 may be a promising NRR electrocatalyst.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
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IF 8.1
Jin-Jian Pan,Jia Huang,Yuan-Hang Qin,Zhen Chen,Li Yang,Cun-Wen Wang,Xingmao Jiang
Ba-based perovskite oxides rich in oxygen vacancies (OVs) are anticipated to possess robust electron-donating capabilities and other favourable properties, rendering them a promising support for Ru catalysts in NH 3 synthesis. Herein, a glucose-urea deep eutectic solvent calcinating method was developed to synthesize an OV-rich BaTiO 3 (BTO-H) support for Ru catalysts. The BTO-H-supported Ru (Ru/BTO-H) catalyst achieves an impressive NH 3 synthesis rate of 5133 μmol g cat –1 h −1 (256.7 mmol g R u –1 h −1 ) at 400 °C and 0.1 MPa, surpassing the performance of Ru catalysts supported on OV-poor BTO supports and other supported Ru catalysts. Physical characterizations and kinetic experiments reveal the multifaceted influence of OVs on enhancing the catalytic performance of Ru/BTO-H in NH 3 synthesis. OVs serve as electron donors to Ru catalyst, facilitating the activation and dissociation of N 2 . Simultaneously, OVs act as hydrogen acceptors from the Ru surface, mitigating hydrogen poisoning effects. Additionally, OVs stimulate the formation of surface hydrides, not only providing active sites for N 2 activation but also bestowing an electron-donating effect on the supported Ru catalyst. The combined positive effects of OVs establish BTO-H as an outstanding support for Ru catalysts in NH 3 synthesis.
研究领域:
材料科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2018
·
IF 6.759
Na Tong,Ying Wang,Yang Liu,Minbo Li,Zizhong Zhang,Huijuan Huang,Tao Sun,Jinxiang Yang,Fuying Li,Xuxu Wang
Photocatalytic ammonia synthesis is of great importance but remains very challenging in photocatalysis. Here, we fabricated a photocatalytic reaction system for the efficiently photocatalytic nitrate reduction to ammonia under UV irradiation using PdSn/NiO/NaTaO 3 :La as a photocatalyst in the presence of formic acid. Several important factors of the photocatalytic performance were investigated, including initial concentration of the nitrate solution, initial pH value and cocatalyst loadings. Nitrate conversion reaches 100% and ammonia selectivity is 72% over the optimum photocatalyst with 5% bimetallic PdSn alloy and 0.2% NiO loadings. The outstanding performance of photocatalyst can be ascribed to both the strong adsorption of nitrite on NiO and the efficient separation of electron-hole pairs by PdSn bimetallic alloy. Besides as the hole scavenger, formic acid also provides not only carboxyl anion radicals for nitrate reduction but also the in-situ buffer effect on ammonia formation. These results give inspiration for designing the reactive system with efficient photocatalytic ammonia synthesis.
研究领域:
材料科学
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环境科学
·
化学工程
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）