Materials Today Energy
·
2021
·
IF 7.311
H. Yu,Z. Wang,W. Tian,Z. Dai,Y. Xu,X. Li,L. Wang,H. Wang
Electrochemical nitrogen reduction reaction (NRR) has been regarded as one of the most promising alternative strategies for nitrogen fixation, and the design of efficient NRR catalysts is the critical factor. Herein, boron and sulfur co-doped mesoporous Rh film on Ni foam (B, S-mRh/NF) is developed for electrochemical ammonia synthesis. The boron and sulfur co-doping, the B, S-mRh/NF, can inhibit competitive hydrogen evolution reaction effectively. Owing to binder-free mesoporous structures, binder-free characteristic, and multicomponent alloy, the B, S-mRh/NF displays a high NH 3 yield of 11.88 μg/h/cm 2 at −0.1 V and Faraday efficiency of 38.42% at −0.05 V in neutral electrolyte. This work offers an effective strategy for the rational design of nonmetal-doped porous Rh electrocatalysts with self-supported structure, which would be highly potential for the electrochemical ammonia synthesis.
研究领域:
化学工程
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材料科学
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电化学
✓ 已验证
DOI
高影响因子
NANOTECHNOLOGY
·
2022
·Vol. 33
·期 38
·385703
·
IF 3.953
Mei Zhang,Lin Cui,Qiqi Mao,Ziqiang Wang,Hongjie Yu,You Xu,Xiaonian Li,Liang Wang,Hongjing Wang
Exploring cost-effective and highly active electrocatalysts is of great significance for sustainable electrochemical NH3 synthesis. Palladium (Pd)-based catalysts have been unanimously considered as one of the most efficient catalysts for the nitrogen reduction reaction (NRR). Herein, self-supported mesoporous Pd film with partial oxidation on Ni foam (mPd-PdO/NF) was synthesized through the micelle-assisted chemical replacement method coupled with air oxidation under 260 °C, and the mPd-PdO/NF electrocatalyst exhibited superior NRR performance with the maximum values of rNH3 (24.8 mg h−1 mgcat.−1) and FE (16.64%) were obtained at −0.1 V, relative to the single counterparts (mPd/NF and mPdO/NF). It is proposed that both metallic Pd and its oxide domains when co-existing with a phase boundary between them can facilitate nitrogen activation and hydrogenation, resulting in an enhanced NRR performance. This work provides an inspiring strategy for the rational design of highly active and durable metal–metal–oxide nanoarchitectonics for ammonia electrosynthesis.
研究领域:
电化学
·
材料科学
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催化
·
可持续化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INORGANIC CHEMISTRY
·
2023
·
IF 4.6
Naiyun Liu,Ruqiang Wu,Yixian Liu,Yunliang Liu,Peiji Deng,Yaxi Li,Yongchao Du,Yuanyuan Cheng,Zechao Zhuang,Zhenhui Kang,Haitao Li
Electrochemical nitrogen reduction reaction (NRR) is a promising method for ammonia synthesis under ambient conditions. However, the NRR performance is limited to an extremely strong N≡N bond in N2 and the competing hydrogen evolution reaction. Introducing oxygen vacancies (OVs) has been considered as a forceful means to accelerate the sluggish NRR reaction kinetics. Herein, we reported the design of Fe-doped NiMoO4 catalysts for NRR. Fe doping can increase the amount of OVs in the catalyst and contribute to lattice strain enhancement, thereby leading to the improvement of the electron transport rate and catalytic active for NRR. In 0.1 M Na2SO4 solution, the 5% Fe-NiMoO4 catalyst achieves a NH3 yield rate of 15.36 μg h–1 mgcat.–1 and a Faradaic efficiency of 26.85% under −0.5 V versus RHE. Furthermore, the 5% Fe-NiMoO4 catalyst exhibits excellent stability (up to 13 h) during the reaction.
研究领域:
材料科学
·
催化
·
电化学
·
化工
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Hongjing Wang,Qiqi Mao,Hongjie Yu,Shengqi Wang,You Xu,Xiaonian Li,Ziqiang Wang,Liang Wang
Electrocatalysis nitrogen reduction reaction (NRR) is expected to achieve sustainable clean and sustainable NH 3 production. Owing to the chemical inertness of N 2 , the design of efficient catalysts is a critical issue. In this work, we propose micelle-assisted replacement method to in situ synthesize mesoporous Au 3 Rh film on Ni foam (mAu 3 Rh/NF). Because of the bimetallic mesoporous and binder-free structures, mAu 3 Rh/NF obtains high Faraday efficiency of 23.84% and NH 3 yield of 26.29 μg h −1 mg -1 cat. for NRR in 0.1 M Na 2 SO 4 at − 0.1 V, outperforming other counterparts with different Au/Rh ratios. This micelle-assisted synthesis method is universal to synthesize high-efficiency mesoporous noble films for NRR and beyond.
研究领域:
材料科学
·
电化学
·
催化
·
可持续化学
✓ 已验证
产品关联
DOI
高影响因子
Energy & Environmental Materials
·
2021
·Vol. 6
·期 1
·e12298
·
IF 15.122
Fanbo Meng,Jiayao Qin,Xingyu Xiong,Xiangjie Li,Renzong Hu
Metal–N 2 battery can be applied in both energy storage and electrochemical nitrogen reduction reaction (NRR); however, there has been only extraordinarily little study on metal–N 2 battery since its electrochemical reversibility still needs further proofs. And its electrochemical performances also need to be enhanced. Herein, we investigated the discharge–charge reactions between Li anode and N 2 cathode via designing an efficient catalyst of nanosized SnO 2 particles dispersed on N-doped carbon nanosheets (SnO 2 @NC) for the Li-N 2 battery, with good cyclic stability and a high specific capacity of 0.25 mA h (~500 mA h g −1 ) at a large current density of 1000 mA g −1 . The electrochemical reversibility of both NRR in the discharge process and nitrogen extraction reaction in the charge process for Li-N 2 battery is discussed. Time-of-flight secondary ion mass spectrometry results imply that the SnO 2 @NC can effectively promote the adsorption of N 2 and the activation of NRR in the discharge process. Furthermore, ex situ X-ray photoelectron spectroscopy and Fourier transform infrared tests are performed to study the electrochemical reversibility of Li-N 2 battery. It can be proved that the formation and decomposition of discharging product Li 3 N are electrochemical reversible during cycling in our deigned Li-N 2 battery system with SnO 2 @NC catalyst.
研究领域:
能量存储
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电化学
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材料科学
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催化
✓ 已验证
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2019
·
IF 5.383
Qiwen Zhang,Yongli Shen,Yufan Hou,Liting Yang,Baili Chen,Zhen Lei,Weiqing Zhang
The composition-activity relationship is highly desirable for electrocatalytic nitrogen reduction reaction (NRR) because it could guide the rational design of efficient NRR catalysts. In this work, the composition effect of Ag-based alloy nanotubes on electrocatalytic NRR activity is systematically investigated. It is found that, among AgAu nanotubes with atomic ratio from 8:1 to 1:2, Ag 2 Au 1 alloy nanotubes achieve the largest enhancement for NRR catalytic activity. Specifically, the NH 3 production rate and faradaic efficiency of Ag 2 Au 1 nanotubes are 21.7 μg h −1 mg cat −1 and 3.8% at −0.30 V vs. RHE, respectively, which were 3.0 and 3.6 times higher than those of Ag nanowires . Compared with Ag 2 Pd 1 and Ag 2 Pt 1 nanotubes, Ag 2 Au 1 hollow nanotubes also exhibit a better NRR catalytic activity. Theoretical calculation results indicate that the negative ion characteristic of Au atoms in the Ag 2 Au 1 alloy is favorable for the adsorption and activation of N 2 . Moreover, Ag 2 Au 1 nanotubes showed stable NH 3 yield rate and faradaic efficiency up to 18 h, revealing its great potential for promising NRR electrocatalysis .
研究领域:
电化学
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催化
·
材料科学
·
纳米技术
✓ 已验证
产品关联
DOI
高影响因子
Nano Energy
·
2021
·
IF 17.881
Cheng Du,Chenglong Qiu,Zhongying Fang,Ping Li,Yijing Gao,Jianguo Wang,Wei Chen
Electrocatalytic nitrogen reduction reaction (NRR), which can produce ammonia from N 2 and H 2 O under ambient conditions, has emerged as a promising sustainable alternative to the Haber-Bosch (H-B) process. However, their unsatisfied conversion efficiency and selectivity severely restrict the real utilization of NRR, owing to the stubborn triple bond in the N 2 molecule and the competitive hydrogen evolution reaction (HER). Here, inspired from the local microenvironment of the nitrogenase, we report for the first time a facile and general strategy to boost the NRR selectivity and activity through the self-assembled monolayer (SAM) of hexanethiol (HEX) on a series of metal electrocatalysts (Cu, Au, Pt, Pd and Ni). Molecular dynamics (MD) simulations suggest that the HEX SAM provides a hydrophobic microenvironment to impede the diffusion and adsorption of water molecules and promote that of N 2 molecules, thus inhibiting HER and simultaneously improving the NRR performance. Notably, among all the prepared samples, the highest Faradic efficiency (FE) of 50.5% is achieved on Cu-HEX with NH 3 formation rate (R) of 1.2 μg h −1 cm −2 . Remarkably, for the HER-favored Pt catalyst, the highest R of 26.4 μg h −1 cm −2 is also achieved on Pt-HEX with FE of 1.8% under 1 cm 2 of electrode area. The present strategy not only represents a general diffusion-controlled method to engineer high-performance NRR electrocatalysts, but also provides a new insight into the effect of surface chemistry of catalysts on the NRR process and kinetics.
研究领域:
电化学
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催化
·
材料科学
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化学工程
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可持续化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2021
·
IF 8.067
Tayiba Ilyas,Fazal Raziq,Nasir Ilyas,Liuxin Yang,Sharafat Ali,Amir Zada,Syedul Hasnain Bakhtiar,Yong Wang,Huahai Shen,Liang Qiao
The electrocatalytic nitrogen reduction reaction (NRR) has emerged as a promising renewable energy source and a feasible strategy as an alternative to Haber-Bosch ammonia (NH 3 ) synthesis. However, finding an efficient and cost-effective robust catalyst to activate and cleave the extremely strong triple bond in nitrogen (N 2 ) for electrocatalytic NRR is still a challenge. Herein, a FeNi@CNS nanocomposite as an efficient catalyst for N 2 fixation under ambient conditions is designed. This FeNi@CNS nanocomposite was prepared by a simple water bath process and post-calcination. The FeNi@CNS is demonstrated to be a highly efficient NRR catalyst, which exhibits better NRR performance with exceptional Faradaic efficiency of 9.83% and an NH 3 yield of 16.52 μg h −1 cm −2 in 0.1 M Na 2 SO 4 aqueous solution. Besides, high stability and reproducibility with consecutive 6 cycles for two hours are also demonstrated throughout the NRR electrocatalytic process for 12 h. Meanwhile, the FeNi@CNS catalyst encourages N 2 adsorption and activation as well as effectively suppressing competitive HER. Therefore, this earth-abundant FeNi@CNS catalyst with a subtle balance of activity and stability has excellent potential in NRR industrial applications.
研究领域:
材料科学
·
电化学
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催化
·
可再生能源
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
H.Y. Zhou,Y.B. Qu,Y.C. Fan,Z.L. Wang,X.Y. Lang,J.C. Li,Q. Jiang
Carbon-free electrocatalytic nitrogen reduction reaction (NRR) offers an environmentally sustainable alternative to the current Haber-Bosch process in the industry. However, this process is still limited by the scaling relations and the competitive hydrogen evolution reaction (HER). Using the density functional theory, we theoretically present a strategy for separating the active sites of the N 2 activation and the hydrogenation of NH z (z = 1, 2) intermediates on the Ni 3 Mo surface, which subtly optimized the adsorption of intermediates and bypasses the scaling relations, achieving efficient NRR with an ultralow limiting potential of − 0.19 V. Besides, the Ni 3 Mo greatly protects the active centers of NRR from competitive H adsorption and retard the undesired HER, enabling highly selective NH 3 synthesis. The above theoretical designs are supported by proof-of-concept experimental results, where Ni 3 Mo exhibits excellent NRR performance with the NH 3 yield rate of 17.35 ± 0.3 μg h −1 cm −2 at − 0.35 V.
研究领域:
化学
·
材料科学
·
电化学
·
催化
✓ 已验证
产品关联
DOI
高影响因子
Inorganic Chemistry Frontiers
·
2023
·Vol. 10
·期 19
·5700-5709
·
IF 7
Yixian Liu,Ruqiang Wu,Yunliang Liu,Peiji Deng,Yaxi Li,Yuanyuan Cheng,Yongchao Du,Zenan Li,Xiong Yan,Naiyun Liu,Zhenhui Kang,Haitao Li
As an environmentally friendly and sustainable method for ammonia synthesis, nitrogen reduction reaction (NRR) by electrocatalysis possesses several advantages, including viability under mild conditions, abundant reaction raw materials and low energy consumption, and thus it is supposed to be a promising alternative to the traditional Haber–Bosch process. However, the stable NN bonds in the nitrogen (N2) and the competing hydrogen evolution reaction (HER) put harsh requirements on catalysts. In this study, the CoS/MoS2 heterojunction catalyst where CoS nanoparticles are anchored on the MoS2 nanosheets is reported as a high-efficiency NRR catalyst. The catalysts have high NH3 yield (23.23 μg h−1 mgcat.−1), reasonable faradaic efficiency (FE, 12.63%) and long-term electrochemical stability under −0.45 V vs. RHE in 0.1 M Na2SO4 solution, whose performance is better than MoS2 and CoS. The TPV results show rapid interfacial electron transfer and good conductivity of the material, and the DFT calculation reveals that the CoS attached to the (100) plane effectively enhances N2 adsorption and catalysis performance.
研究领域:
材料科学
·
电化学
·
催化
·
可持续化学
✓ 已验证
产品关联
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2024
·
IF 5.5
Daming Feng,Lixue Zhou,Chang Liu,Hui Li,Yusheng Zhang,Yali Yao,Tianyi Ma
Electrocatalytic nitrogen reduction reaction (NRR) for the synthesis of ammonia (NH 3 ) is one of the green and mild methods of artificial nitrogen fixation, promising as an alternative to replace the existing industrial process. Under the requirements of green chemistry and sustainable development, the design and development of highly active and stable electrocatalysts is very important for improved synthesis performance. Mimicking from the natural nitrogenase, Fe and Mo based catalysts have attracted much attention due to their superior catalytic performance for N 2 adsorption and activation. In this work, an interfacial engineering strategy has been used to prepare a Fe, Mo-bimetallic electrocatalyst for the electrosynthesis of NH 3 . In detail, the pre-pyrolyzed biochar-based Fe 2 O 3 composites were decorated with nano-flowered MoS 2 /MoO 2 hybrids by a solvothermal process (MoS 2 /MoO 2 @Fe 2 O 3 /BC). As confirmed by the extensive characterization, the further modification not only introduced functional counterparts into the electrocatalysts but also regulated the morphology of the nanostructure. The electrochemical tests showed that the highest NH 3 yield rate of MoS 2 /MoO 2 @Fe 2 O 3 /BC was 4.87 μg h − 1 cm −2 and highest FE was 16.5% in 0.1 M Na 2 SO 4 . The catalytic stability and durability were also presented in the longtime electrolysis and cycling experiments. The improved catalytic performance of decorated catalyst, as evidenced by the comparison with Fe 2 O 3 /BC, is attributed to the increased electrocatalytic active area, the moderated hydrophilicity, and the synergistic effect of Fe, Mo-bimetallic active sites. This study provides a new perspective for the design and development of low-cost transition metal complexes as electrocatalysts for nitrogen reduction reactions.
研究领域:
电化学
·
催化
·
材料科学
·
环境化学
·
可持续能源
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）