Sustainable Energy & Fuels
·
2020
·Vol. 4
·期 7
·3334-3339
·
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
·
电化学
·
催化
·
能量转换
✓ 已验证
产品关联
DOI
高影响因子
Inorganic Chemistry Frontiers
·
2021
·Vol. 8
·期 13
·3336-3341
·
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
·
电化学
·
材料科学
·
化工
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2020
·
IF 16.683
Jinxiu Zhao,Xuejing Liu,Xiang Ren,Xu Sun,Dongxu Tian,Qin Wei,Dan Wu
Electrochemical N 2 reduction is developing as an appealing carbon-neutral strategy for NH 3 artificial synthesis but seriously influenced by requiring high-efficiency electrocatalysts for the N 2 activation at ambient conditions. Here, we reported that defective-rich ZnS nanoparticles supported on reduced graphene oxide (DR ZnS-rGO) acts as a high-efficiency electrocatalyst for ambient N 2 -to-NH 3 conversion with excellent selectivity. In 0.1 M HCl, such DR ZnS-rGO presents a large NH 3 yield of 51.2 μg h –1 mg cat. –1 (−0.15 V vs . reversible hydrogen electrode, RHE) and a high faradic efficiency of 28.2 % (−0.10 V vs . RHE), as well as high electrochemical and structure stability. Isotopic labelling samples experiments reveal that the synthetic NH 3 directly arise from the supplied N 2 . Density functional theory calculations demonstrated that the engineering S vacancies in DR ZnS-rGO not only provide reaction sites for N 2 -to-NH 3 conversion but activate of N 2 molecules.
研究领域:
材料科学
·
电化学
·
催化
·
化学工程
✓ 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）