JOURNAL OF SOLID STATE CHEMISTRY
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2022
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IF 3.656
Lijun Guo,Feifei Li,Jianxin Liu,Rui Li,Zhuobin Yu,Qing Xi,Lulu Zhang,Yaru Li,Caimei Fan
Morphology regulation is a simple way to improve photocatalytic activity. In this work, a MIL-101(Fe) photocatalyst with cracked spindle morphology has been successfully prepared by EG pre-coordination solvothermal method . The cracking degree of MIL-101(Fe) can be regulated by adjusting pre-coordination time. The MIL-101(Fe) with the optimal uniform crack displays a best NH 3 evolution rate of 592 μmol h −1 g −1 under the visible light irradiation . Cracked MIL-101(Fe) is similar to a semi-exposed model, which can increase the number of reactive sites, improve refraction and reflection of light, and ultimately enhance the photocatalytic nitrogen fixation activity. This work developed a convenient strategy to improve the photocatalytic activity of nitrogen reduction by controlling morphology.
研究领域:
材料科学
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环境科学
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化学工程
✓ 已验证
DOI
高影响因子
Nanoscale
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2019
·Vol. 12
·期 3
·1811-1816
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IF 6.97
Yongqin Liu,Liang Huang,Xinyang Zhu,Youxing Fang,Shaojun Dong
The electrochemical nitrogen reduction reaction (NRR) under ambient conditions is currently attracting intense attention, but it still remains a great challenge to develop highly selective and active NRR electrocatalysts. Inspired by the intrinsic NRR activity of Au, we systematically studied the synergistic enhanced effect of incorporating other transition metals into Au on its NRR activity. A general strategy was used to synthesize a series of Au-based bimetallic nanocatalysts (AuCu, AuAg, AuPd and AuRu), and the NRR catalytic performance of the as-obtained electrocatalysts was investigated in detail. The experimental results indicate that the positive effect of Cu on NRR was the most remarkable in comparison with that of Ag, Ru and Pd, which can be ascribed to the synergy of the Au and Cu components via modulating the electronic structure and further changing the binding affinity of adsorbed N atoms on the catalyst. Finally, the optimized nanocatalyst with the atom ratio of Au1Cu1 achieved the highest faradaic efficiency (54.96%) and ammonia yield rate (154.91 μg h−1 mgcat−1) at −0.2 V vs. RHE, exceeding those of the previously reported Au nanocatalysts.
研究领域:
材料科学
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电化学
✓ 已验证
DOI
高影响因子
ELECTROCHIMICA ACTA
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2021
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IF 6.901
Jiankun Wei,Yidan Jing,Zelin Zhao,Zhengwen Fan,Zijia Liang,Junling Huang,Han Wu,Zhizhong Xie,Dan Liu,Deyu Qu,Haolin Tang,Junsheng Li
Electrochemical nitrogen reduction reaction (ENRR) is a promising supplement to the existing Haber-Bosch process due to its mild reaction condition and high theoretical efficiency. However, rational design of efficient ENRR catalyst remains to be the key challenge for the future development of practical ENRR process. In this work, we propose a strategy to enhance the performance of ENRR catalyst by catalyst-support interactions. This strategy is verified with Au/ZrO 2 catalyst. Both experimental and theoretical investigations show that electron is transferred from ZrO 2 substrate to Au. Such an electron transfer process modifies the electronic structure of Au, which enhances the ENRR activity HER performance of the Au active components. Benefiting from the catalyst-support interactions, the optimal Au/ZrO 2 catalyst shows a high ammonia yield of 54.84 μg h −1 mg −1 Au .
研究领域:
材料科学
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电化学
✓ 已验证
DOI
高影响因子
Nano Research
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2024
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IF 9.5
Liu Dong-Xue,Deng Xin,Zhu Yong-Fu,Meng Zhe,Sun Xue-Feng,Shi Miao-Miao,Zhong Hai-Xia,Yan Jun-Min
Electrocatalytic reduction of nitrate \(({\rm{N}}{{\rm{O}}_3}^ - )\) and nitride \(({\rm{N}}{{\rm{O}}_2}^ - )\) to ammonia (NH 3 ) is of wide interest as a promising alternative to the energy-intensive Haber-Bosch route for mitigating the vast energy consumption and the accompanied carbon dioxide emission, as well as benefiting for the relevant sewage treatment. However, exploring an efficient and low-cost catalyst with high atomic utilization that can effectively facilitate the slow multi-electron transfer process remains a grand challenge. Herein, we present an efficient hydrogenation of \({\rm{N}}{{\rm{O}}_3}^ - /{\rm{N}}{{\rm{O}}_2}^ - \) species to NH 3 in both alkaline and neutral environments over the Fe 2 (MoO 4 ) 3 derived hybrid electrocatalyst with the metallic Fe site on FeMoO 4 (Fe/FeMoO 4 ). The Mo ingredient can play a synergistically positive role in further promoting the NH 3 production on Fe. As a result, Fe/FeMoO 4 behaves well in the electrochemical NH 3 generation from \({\rm{N}}{{\rm{O}}_2}^ - \) with a maximum NH 3 Faradaic efficiency (FE) of 96.53% and 87.68% in alkaline and neutral electrolyte, corresponding to the NH 3 yield rate of 640.68 and 302.56 \({\rm{mg}} \cdot {{\rm{h}}^{ - 1}} \cdot {\rm{m}}{{\rm{g}}_{{\rm{cat}}.}}^{ - 1}\) , respectively, which outperforms the Fe and Mo counterpart and other similar catalyst, showing the robust catalytic capacity of each active site.
研究领域:
催化
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电化学
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环境科学
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材料科学
✓ 已验证
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2024
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IF 10.8
Yongguang Bu,Wenjing Yu,Qiang Yang,Wenkai Zhang,Qingyu Sun,Wensu Wu,Peixin Cui,Chao Wang,Guandao Gao
Electroreduction of nitrate (NO3RR) to ammonia in membraneless electrolyzers is of great significance for reducing the cost and saving energy consumption. However, severe chemical crossover with side reactions makes it challenging to achieve ideal electrolysis. Herein, we propose a general strategy for efficient membraneless ammonia synthesis by screening NO3RR catalysts with inferior oxygen reduction activity and matching the counter electrode (CE) with good oxygen evolution activity while blocking anodic ammonia oxidation. Consequently, screening the available Co–Co system, the membraneless NO3–-to-NH3 conversion performance was significantly higher than H-type cells using costly proton-exchange membranes. At 200 mA cm–2, the full-cell voltage of the membraneless system (∼2.5 V) is 4 V lower than that of the membrane system (∼6.5 V), and the savings are 61.4 kW h (or 56.9%) per 1 kg NH3 produced. A well-designed pulse process, inducing reversible surface reconstruction that in situ generates and restores the active Co(III) species at the working electrode and forms favorable Co3O4/CoOOH at the CE, further significantly improves NO3–-to-NH3 conversion and blocks side reactions. A maximum NH3 yield rate of 1500.9 μmol cm–2 h–1 was achieved at −0.9 V (Faraday efficiency 92.6%). This pulse-coupled membraneless strategy provides new insights into design complex electrochemical synthesis.
研究领域:
电化学
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催化
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能源效率
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
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