CHINESE JOURNAL OF CATALYSIS
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2026
·
IF 17.2
Fengjuan Guo,Chunyao Ma,Yue Huang,Sitong Hang,Junwei Ma,Hongtao Gao
Electrocatalytic nitrogen reduction reaction (NRR) under ambient conditions offers a sustainable alternative to the energy-intensive Haber-Bosch process. However, the two canonical catalytic pathways face intrinsic limitations: the alternating mechanism suffers from high *NH 2 NH 2 desorption losses, while the distal pathway requires prohibitive activation energy for N 2 protonation. The simultaneous realization of high activity and selectivity thus remains a critical challenge. Here, we demonstrate that boron doping modulates the electronic structure of Mo 2 TiC 2 T x /MoO 2 by upshifting the d -/ p -band center toward the Fermi level, unveiling the dominant a hybrid “distal-alternating” pathway that favors the *NNHH → *NHNH 2 transition rather than the *NNHH → *N cleavage. In addition, the electron-deficient B sites weaken the binding affinity toward Lewis-acidic protons under acidic conditions, thereby effectively suppressing the competing hydrogen evolution reaction. Significant interfacial charge transfer from MoO 2 to the B@Mo 2 TiC 2 T x surface further ensures a sufficient electron supply for N 2 activation and stepwise hydrogenation. As a result, B@Mo 2 TiC 2 T x /MoO 2 delivers an impressive ammonia yield of 121.18 μg h −1 mg cat. −1 with a Faradaic efficiency of 75.94% at a mild potential of –0.2 V vs . RHE. This work unveils the mechanistic feasibility of a non-classical hybrid NRR pathway and establishes a rational strategy for designing next-generation high-efficiency nitrogen reduction electrocatalysts.
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DOI
高影响因子
Functional Materials Letters
·
2023
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IF 1.3
Meiqi Zhai,Yajie Bai,Xia Li,Fengfeng Wang,Wei-Qiang Fan,Hongye Bai
Photoelectrochemical reduction of nitrate (PEC NRR) to ammonia (NH 3 ) is a promising means with water as hydrogen source under room temperature. The construction of photoelectrode with efficient light response and reaction kinetics is the core point to achieve high NH 3 yield efficiency. Herein, a cerium-based metal organic framework (Ce-MOF) was successfully decorated on the copper phthalocyanine (CuPc). The CuPc/Ce-MOF heterostructure exhibits the ideal nitrate catalytic reduction activity, and the NH 3 yield (−0.6 V versus RHE) increases to 1.58 μ g h − 1 cm − 2 from 0.67 μ g h − 1 cm − 2 (CuPc). Besides, the cycle experiments reveal that the CuPc/Ce-MOF heterostructure has maintained good catalytic stability. This work explores the PEC NRR process mechanism of CuPc/Ce-MOF samples and provides a new idea for green NH 3 production.
研究领域:
材料科学
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电化学
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光化学
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催化
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DOI
高影响因子
Nanoscale
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2020
·Vol. 12
·期 25
·13507-13512
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IF 6.895
Hongjing Wang,Songliang Liu,Hugang Zhang,Shuli Yin,You Xu,Xiaonian Li,Ziqiang Wang,Liang Wang
Electrochemical nitrogen reduction reaction (NRR) provides a facile and sustainable route to synthesize ammonia. The preparation of efficient and high-performance catalysts is one of the most important issues in large-scale applications of the electrochemical synthesis of ammonia. Herein, we have devised a simple method to fabricate three-dimensional palladium-silver-sulphur porous nanosponges (Pd–Ag–S PNSs) under room temperature. The porous network can provide more active sites and accessible channels for the reaction species. The incorporation of sulfur reduces the energy barrier of NRR and promotes the nitrogen hydrogenation to ammonia. Intrinsically, the Pd–Ag–S PNSs demonstrates a superior NRR performance with an NH3 yield of 9.73 μg h−1 mg−1cat. and a faradaic efficiency of 18.41% at −0.2 V, superior to those of the undoped Pd–Ag PNSs. The design of the three-dimensional metallic nanosponges with the doping of nonmetallic elements is a highly valuable strategy for NRR and other electrocatalytic reactions.
研究领域:
材料科学
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催化
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电化学
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DOI
PubMed
高影响因子
Journal of Materials Chemistry A
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2019
·Vol. 7
·期 20
·12526-12531
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IF 10.733
Hongjie Yu,Ziqiang Wang,Dandan Yang,Xiaoqian Qian,You Xu,Xiaonian Li,Hongjing Wang,Liang Wang
The electrochemical nitrogen reduction reaction (NRR) is considered as a facile and sustainable strategy for ammonia production. Design of high-performance electrocatalysts is the crucial issue for the NRR. Herein, we present a one-pot reduction method to directly synthesize bimetallic Ag3Cu porous networks (Ag3Cu BPNs). Owing to their porous networks and bimetallic composition, the Ag3Cu BPNs exhibit outstanding NRR performance with a high NH3 yield of 24.59 μg h−1 mgcat.−1 and faradaic efficiency of 13.28% at −0.5 V vs. the reversible hydrogen electrode. This study proposes a facile and scalable route for the development of metallic porous networks with an interconnected structure and desired components for electrochemical ammonia production.
研究领域:
电化学
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材料科学
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催化
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可持续化学
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DOI
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2021
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IF 4.464
Qiqi Mao,Chunjie Li,Wenjing Tian,Tongqing Zhou,You Xu,Ziqiang Wang,Xiaonian Li,Liang Wang,Hongjing Wang
Electrochemical nitrogen reduction reaction (NRR) is a facile and sustainable alternative strategy to Haber-Bosch process for ammonia synthesis. Design of efficient and stable electrocatalysts is critical to NRR. Herein, a two-step method is proposed to fabricate surface Se-doping mesoporous Rh nanoparticles (Se-mRh NPs). Owing to the mesoporous structure and Se modified surface, the Se-mRh NPs exhibit a superior NH 3 yield (21.36 μg h −1 mg −1 cat. ) and Faradaic efficiency (34.54 %) in a neutral electrolyte (0.1 M Na 2 SO 4 ) relative to mesoporous Rh nanoparticles (mRh NPs). The presented synthetic approach is very valuable for design of metallic catalysts with Se modified surface for various electrocatalytic applications.
研究领域:
材料科学
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电化学
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催化
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DOI
高影响因子
Journal of Materials Chemistry A
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2020
·Vol. 8
·期 18
·8920-8926
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IF 11.301
Ying Liu,Xiaorong Zhu,Qinghua Zhang,Tang Tang,Yun Zhang,Lin Gu,Yafei Li,Jianchun Bao,Zhihui Dai,Jin-Song Hu
The development of efficient and cost-effective electrocatalysts is essential for the electrochemical reduction of N2 to produce NH3 under ambient conditions. Herein, various well-dispersed Mo-based nanoparticles are selectively synthesized to reveal the influences of the compositions and hetero-interfaces on the performance for the N2 reduction reaction (NRR). Systematic experiments discovered that compared with single-component Mo2C or Mo nanoparticles, the heterostructured binary MoC/Mo2C and ternary Mo/MoC/Mo2C nanoparticles exhibit significantly enhanced NRR performance by creating abundant hetero-interfaces. Moreover, theoretical calculations reveal that the integration of metallic Mo with MoC/Mo2C appreciably reduces the energy demand for NH3 desorption, contributing to the enhanced NRR process. As a result, a remarkable NH3 yield rate of up to 20.4 μg h−1 mg−1 and a FE up to 18.9% can be achieved. These findings suggest that engineering crystalline phases and hetero-interfaces represents a new avenue for advancing the electrocatalytic performance of a NRR catalyst.
研究领域:
材料科学
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电化学
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催化
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DOI
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2021
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IF 4.464
Yijun Li,Liangyu Ma,Yaxuan Fu,Cai Zhang,Yanfeng Shi,Yuanhong Xu,Jinghong Li
The electrochemical nitrogen reduction reaction is a more ecologically friendly alternative to the high-energy Haber-Bosch method for ammonia manufacturing, but was lack of efficient catalyst, especially in the neutral electrolyte. Inspired by the composition of biological nitrogenase with the elements of Mo, Fe and S, vulcanized FeMoO 4 was designed as the nitrogen reduction electrocatalyst, which exhibited excellent catalytic performance and stability for nitrogen reduction reaction (NRR) in neutral media. During the NRR test, the vulcanized FeMoO 4 achieved 31.93 μg h - 1 mg cat. -1 ammonia production rate and high Faradaic efficiency (30.9%) at −0.39 V versus the reversible hydrogen electrode (RHE) in 0.1 M Na 2 SO 4 . The results demonstrated the viability of Fe-Mo base as an electrocatalyst for NRR and laid the path for the creation of a nitrogenase-like biomimetic electrocatalysts to achieve the effective N 2 fixation.
研究领域:
电化学
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催化
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材料科学
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环境科学
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DOI
高影响因子
Small
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2019
·Vol. 15
·期 6
·1804769
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IF 10.856
Hongjing Wang,Hongjie Yu,Ziqiang Wang,Yinghao Li,You Xu,Xiaonian Li,Hairong Xue,Liang Wang
Electrochemical reduction of N 2 to NH 3 provides an alternative strategy to replace the industrial Haber–Bosch process for facile and sustainable production of NH 3 . The development of efficient electrocatalysts for the nitrogen reduction reaction (NRR) is highly desired. Herein, a micelle-assisted electrodeposition method is presented for the direct fabrication of porous Au film on Ni foam (pAu/NF). Benefiting from its interconnected porous architectonics, the pAu/NF exhibits superior NRR performance with a high NH 3 yield rate of 9.42 µg h −1 cm −2 and a superior Faradaic efficiency of 13.36% at −0.2 V versus reversible hydrogen electrode under the neutral electrolyte (0.1 m Na 2 SO 4 ). The proposed micelle-assisted electrodeposition strategy is highly valuable for future design of active NRR catalysts with desired compositions toward various electrocatalysis fields.
研究领域:
电化学
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催化
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材料科学
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可持续化学
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产品关联
DOI
PubMed
高影响因子
Sustainable Energy & Fuels
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2020
·Vol. 4
·期 7
·3334-3339
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IF 5.503
You Xu,Tianlun Ren,Shanshan Yu,Hongjie Yu,Shuli Yin,Ziqiang Wang,Xiaonian Li,Liang Wang,Hongjing Wang
The electrocatalytic nitrogen reduction reaction (NRR) for ammonia (NH3) synthesis is highly desirable yet still challenging. Catalysts, as the core component of electrocatalytic NRR systems, are a specific focus of research. In this work, we demonstrate that NRR active semimetal bismuth (Bi) ultrathin nanosheets (Bi NSs) could be prepared by means of the in situ electrochemical reduction-assisted exfoliation of BiOCl nanoplates (BiOCl NPs). Such a conversion, from semiconductive BiOCl NPs to semimetal Bi NSs, could create enlarged surface areas and bring about abundant under-coordinated Bi sites and accelerated electron transport capability. With these advantageous properties, the as-converted Bi NSs exhibit efficient NRR electrocatalytic activity in 0.1 M Na2SO4, achieving a high faradaic efficiency (14.14%) and NH3 yield (11.11 μg h−1 mgcat.−1) at −0.5 V (vs. reversible hydrogen electrode), as well as high NH3 selectivity.
研究领域:
材料科学
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电化学
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催化
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能量转换
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产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
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2019
·
IF 8.456
Hongjie Yu,Ziqiang Wang,Shuli Yin,Chunjie Li,You Xu,Xiaonian Li,Liang Wang,Hongjing Wang
As a promising alternative approach to industrial N2 fixation process, electrocatalytic N2 reduction reaction (NRR) can achieve efficient, sustainable, and eco-friendly ammonia production under ambient conditions. Developing efficient NRR catalysts is critical for the electrochemical ammonia synthesis. Herein, self-supported mesoporous Au3Pd film on Ni foam (mAu3Pd/NF) has been in situ synthesized via a micelle-assisted replacement strategy. Combination of bimetallic compositions, interconnected mesoporous structure, and binder-free characteristic, the mAu3Pd/NF shows a superior NRR performance in 0.1 M Na2SO4. This micelle-assisted replacement route is very important to construct efficient self-supporting mesoporous films for the NRR and other fields.
研究领域:
材料科学
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电化学
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催化
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可持续化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Inorganic Chemistry Frontiers
·
2021
·Vol. 8
·期 13
·3336-3341
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IF 6.569
Hongxi Zhang,Zengyao Wang,Jianfeng Shen,Mingxin Ye
The electro-catalytic nitrogen reduction reaction (NRR) at room temperature and atmospheric pressure has great potential in NH3 production, but the low product yield because of the low density of active sites and slow reaction kinetics greatly limits its further development. To overcome these shortcomings, a series of nano PdxCuy bimetal catalysts with adjustable Pd/Cu atomic ratios were prepared and used as electrocatalysts in the NRR. The PdxCuy bimetal catalysts possess large surface area and numerous active sites. In particular, due to excellent conductivity and reactivity, the Pd3Cu bimetallic catalyst showed remarkable performance with a NH3 yield of 22.9 μg h−1 mgcat−1 and a faraday efficiency (FE) of 3.26% at an overpotential of −0.25 V, while the PdCu3 bimetal catalyst exhibited a high FE of 15.62% and a NH3 yield of 19.1 μg h−1 mgcat−1. Moreover, even at a lower overpotential of −0.15 V, the NRR yield was far more than 10 μg h−1 mgcat−1. Thus, this strategy and study for preparing bimetal catalysts with adjustable FE would be beneficial for the preparation of superior bimetal NRR catalysts.
研究领域:
催化
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电化学
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材料科学
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化工
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
·
IF 19.503
Hong Yu Zhou,Yan Bin Qu,Jian Chen Li,Zhi Li Wang,Chun Cheng Yang,Qing Jiang
Carbon-free electrocatalytic nitrogen reduction reaction (NRR) is an attractive replacement of the current Haber-Bosch method. However, there is a lack of suitable electrocatalysts that simultaneously achieve both high activity and selectivity, hindering the practical applications of NRR. Herein we theoretically design an electron-deficient surface of MoB 2 for preferential N 2 adsorption and thus increase the local concentration of N 2 around the active sites. These lead to outstanding NRR selectivity that can evidently retard the competing HER even at the NRR operating potential. The corresponding theoretical limiting potential for NRR is as low as − 0.34 V. Our proof-of-concept experiment confirms the above theoretical design, in which excellent NRR performances (NH 3 yield rate of ~ 40.94 μg h −1 mg −1 , FE of ~ 30.84%) have been achieved. The strategy of inducing electron deficiency on active sites provides new insight into the rational design of NRR electrocatalysts for realizing green and effective ammonia synthesis in practical applications.
研究领域:
材料科学
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化学工程
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催化
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电化学
✓ 已验证
产品关联
DOI
高影响因子
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