Journal of Physical Chemistry C
·
2021
·
IF 4.126
Hanxue Yan,Wenbo Gao,Qianru Wang,Yeqin Guan,Sheng Feng,Han Wu,Qing Guo,Hujun Cao,Jianping Guo,Ping Chen
Palladium (Pd) has long been known to be inactive for dinitrogen activation and hence has received little attention for ammonia synthesis. Herein, we report that the reactivity of Pd is changed when reacting with lithium hydride (LiH) forming a series of lithium palladium hydrides such as LiPdH0.7 and Li2PdH2 (denoted as [Li–Pd–H]). LiPdH0.7 promotes N2 fixation by LiH forming Li2NH and LiPd, and the subsequent hydrogenation of Li2NH and LiPd leads to ammonia and regeneration of LiH and [Li–Pd–H]. Based on these experimental results, an ammonia loop mediated by a [Li–Pd–H]–LiH and LiPd–Li2NH composite pair is proposed and demonstrated. An ammonia production rate of 693 μmolNH3 g–1 h–1 was achieved at 300 °C and 1 bar, which is ca. 7 times that of the neat LiH/Li2NH pair at 350 °C and 1 bar and 2 times that of the thermocatalytic process catalyzed by Ru/MgO at 300 °C and 10 bar.
研究领域:
化学
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催化
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材料科学
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Riqing Yan,Hanle Yin,XiFeng Zuo,Weihua Peng,Xiaofeng Zhu,Lei Shi,Jianhua Hou,Dan Wang,Fenghui Ye,Jing Li,Baoguang Mao,Chuangang Hu
Electrocatalytic reduction of nitrate (NO 3 – ) to ammonia (NH 3 ) emerges as a sustainable approach for both wastewater treatment and NH 3 synthesis. Herein, we report a hollow-structured PdCuCo medium-entropy alloy supported on reduced graphene oxide (HPdCuCo/RGO) as an efficient and robust electrocatalyst for nitrate reduction reaction (NO 3 – RR). A unique proton-mediator boosted tandem electrocatalysis toward NH 3 production is established on the HPdCuCo/RGO, where Cu sites promote the NO 3 – -to-NO 2 – conversion, the Co sites facilitate the NO 2 – -to-NH 3 conversion, and the Pd sites serve as proton mediators to further boost the tandem catalysis. As a result, the HPdCuCo/RGO exhibit high performance towards NO 3 – RR in Ar-saturated 0.5 M K 2 SO 4 electrolyte with 2000 ppm NO 3 – , achieving a NH 3 -Faradaic Efficiency of ∼100 % and a corresponding NH 3 yield of 36 mg h –1 mg –1 cat. at −0.5 V versus reversible hydrogen electrode. This study showcases the significant potential of medium-entropy alloys as efficient catalysts for NO 3 – RR, motivating further exploration into the hitherto underexplored domain of medium-entropy alloys for NO 3 – RR.
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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环境科学
✓ 已验证
产品关联
DOI
高影响因子
Small
·
2022
·Vol. 18
·期 23
·2201200
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IF 15.153
Peng Jing,Peixin Liu,Minghao Hu,Xuan Xu,Baocang Liu,Jun Zhang
Electrochemical nitrogen reduction powered by renewable electricity is a promising strategy to produce ammonia. However, the lack of efficient yet cheap electrocatalysts remains the biggest challenge. Herein, hybrid Cu 2 O-CeO 2 -C nanorods are prepared on copper mesh through a metal-organic framework template route. The Cu-loaded Ce-MOF is thermally converted to Cu 2 O-CeO 2 heterojunctions with interfacial Cu-[O X ]-Ce structures embedded in carbon. Theoretical calculations reveal the lower formation energy of oxygen vacancies in Cu-[O X ]-Ce structures than in the Cu 2 O or CeO 2 phase. The Cu-[O X ]-Ce structures with oxygen vacancies enable the formation of interfacial electron-rich Cu(I) species which show significantly enhanced performance toward electrocatalytic nitrogen reduction with an NH 3 yield of 6.37 × 10 −3 µg s −1 cm −2 and a Faradaic efficiency of 18.21% in 0.10 m KOH at −0.3 V versus reversible hydrogen electrode. This work highlights the importance of modulation of charge distribution of Cu-based electrocatalysts to boost the activity toward nitrogen reduction.
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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可再生能源
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Particuology
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2022
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IF 3.251
Hengyuan Liu,Xingjiang Wu,Jianhong Xu
Electrocatalytic nitrogen reduction reaction (NRR) is regarded as a potential routine to achieve environment-friendly ammonia production, because of its abundant nitrogen resources, clean energy utilization and flexible operation. However, it is hindered by low activity and selectivity, in which condition well-designed catalysts are urgently in need. In this work, a binary Mo/Ir nanodots/carbon (Mo/Ir/C) hetero-material is efficiently constructed via microfluidic strategy, of which the nanodots are homogeneously distributed on the carbon skeleton and the average size is approximately 1 nm. Excellent performance for NRR is obtained in 1 mol L −1 KOH, of which the optimized ammonia yield and faradic efficiency are 7.27 μg h −1 cm −2 and 2.31% respectively. Moreover, the optimized ammonia yield of 6.20 μg h −1 cm −2 and faradic efficiency of 10.59% are also obtained in 0.005 mol L −1 H 2 SO 4 . This work achieves the continuous-flow synthesis and controllable adjustment of hetero-materials for favorable morphologies, which provides an innovative pathway for catalyst design and further promotes the development of ammonia production field.
研究领域:
材料科学
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化学工程
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电化学
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催化
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
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2019
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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
Catalysis Science & Technology
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2020
·Vol. 10
·期 5
·1336-1342
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IF 5.721
Ziqi Zhang,Kaida Yao,Linchuan Cong,Zhuochen Yu,Lina Qu,Weimin Huang
Ammonia is one of the most important agricultural fertilizers and renewable energy carriers, and is also one of the most highly produced inorganic compounds in the world. The traditional industrial ammonia synthesis mainly uses the Haber–Bosch method, which consumes a large amount of fossil fuels and emits a lot of greenhouse gas. Thus, a more environmentally friendly method is needed for the production of ammonia. In this paper, we present a new electrocatalyst to produce NH3 under ambient conditions, which was obtained via the carbonization of Ru-dispersed ZIF-8. As a result, the catalyst could achieve a maximum NH3 production rate of about 16.68 μgNH3 h−1 mgcat.−1 at −0.4 V (vs. RHE) and a faradaic efficiency of 14.23% at −0.3 V (vs. RHE) at room temperature and ambient pressure in 0.1 M KOH. Also, the loading of Ru is only 16 wt%. Thus, this work provides a feasible method to design highly dispersed noble metal electrocatalysts for the nitrogen reduction reaction (NRR).
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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可持续化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
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2021
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IF 9.229
Yi Jia,Yi-Gang Ji,Qi Xue,Fu-Min Li,Guang-Tao Zhao,Pu-Jun Jin,Shu-Ni Li,Yu Chen
The nitrate electroreduction reaction (NO3–-ERR) is an efficient and green approach for nitrate remediation, which requires a highly active and selective electrocatalyst. In this work, porous and amorphous cobalt phosphide nanoshuttles (CoP PANSs) are successfully synthesized by using Mg2+ ion-doped calcium carbonate nanoshuttles (Mg-CaCO3 NSs) as the initial reaction precursor via precipitation transformation and a high-temperature phosphidation strategy. Various physical characterizations show that CoP PANSs have porous architecture, amorphous crystal structure, and big surface area. Electrochemical measurements reveal for the first time that CoP PANSs have outstanding electroactivity for NO3–-ERR in a neutral electrolyte. At an applied potential of −0.5 V vs reversible hydrogen electrode, CoP PANSs can achieve a high Faraday efficiency (94.24 ± 2.8%) and high yield rate (19.28 ± 0.53 mg h–1 mgcat–1) for ammonia production, which exceeds most reported values at various electrocatalysts for NO3–-ERR. Thus, the present result indicates that cobalt phosphide nanomaterials have promising application for NO3–-ERR.
研究领域:
材料科学
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电化学
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环境科学
✓ 已验证
产品关联
DOI
PubMed
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
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DOI
高影响因子
Nano Research
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2021
·Vol. 15
·期 2
·972-977
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IF 8.897
Wen Guilai,Liang Jie,Liu Qian,Li Tingshuai,An Xuguang,Zhang Fang,Alshehri Abdulmohsen Ali,Alzahrani Khalid Ahmed,Luo Yonglan,Kong Qingquan,Sun Xuping
Industrial-scale ammonia (NH 3 ) production mainly relies on the energy-intensive and environmentally unfriendly Haber-Bosch process. Such issue can be avoided by electrocatalytic N 2 reduction which however suffers from limited current efficiency and NH 3 yield. Herein, we demonstrate ambient NH 3 production via electrochemical nitrite (NO 2 − ) reduction catalyzed by a CoP nanoarray on titanium mesh (CoP NA/TM). When tested in 0.1 M PBS (pH = 7) containing 500 ppm NO 2 − , such CoP NA/TM is capable of affording a large NH 3 yield of 2,260.7 ± 51.5 µg·h −1 ·cm −2 and a high Faradaic efficiency of 90.0 ± 2.3% at −0.2 V vs. a reversible hydrogen electrode. Density functional theory calculations reveal that the potential-determining step for NO 2 − reduction over CoP (112) is *NO 2 → *NO 2 H.
研究领域:
化学工程
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电化学
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催化
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF SOLID STATE CHEMISTRY
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2025
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IF 3.5
Fang-Ting Wang,Qing-Yun Xie,Huan Jiao,Ling Xu
The accumulation of nitrate/nitrite (NO x – ) in wastewater poses a threat on ecological safety. Electrocatalytic NO x – reduction to ammonia (NO x – RR) is feasible to realize green ammonia production. This work developed a 2D copper metal-organic framework of Cu-BDC (H 2 BDC = 1,4-benzene dicarboxylic acid) as an efficient electrocatalyst for NO x – RR, exhibiting high-performance with the NH 3 yield of 71.20 μmol‧h −1 ‧cm −2 and a Faraday efficiency of 80.9 % at −0.746 V ( vs. RHE) for NO 2 − RR, and the NH 3 yield of 130.16 μmol‧h −1 ‧cm −2 and a Faraday efficiency of 67.42 % at −0.946 V ( vs. RHE) for NO 3 − RR. Isotope labelled 14 NO 3 − and 15 NO 3 − produced 14 NH 4 + and 15 NH 4 + , supporting the formation of NH 3 comes from the NO 3 − RR. In three NO x – RR cycles, all NH 3 yields and Faraday efficiencies show a slight change, demonstrating an excellent electrocatalytic stability in NO x – RR. Our work provides a new material platform for the elimination of nitrate and nitrite through electrocatalytic reduction.
研究领域:
电化学
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环境科学
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催化
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材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
ELECTROCHIMICA ACTA
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2022
·
IF 7.336
Luyun Yang,Jingsha Li,Feng Du,Jingfeng Gao,Hui Liu,Shunyuan Huang,Hehe Zhang,Changming Li,Chunxian Guo
Developing low-cost and high-performance electrocatalysts for electrochemical nitrate reduction to ammonia (NRA) is of great importance to alleviate increasingly energy demand and environmental pollution. Cu electrodes have been widely explored towards NRA, while high overpotential is always required and ammonia selectivity is relatively low. Herein, Ce-doping Cu electrode is designed and fabricated via electrochemical deposition strategy and its electrocatalytic NRA in alkaline conditions is investigated. Effect of the Ce content on the performance of the Ce-doped Cu electrodes are studied, showing that the Cu 10 Ce 10 demonstrates the best performance. It achieves a high ammonia yield rate of 0.99 mmol h −1 cm −2 , Faradaic efficiency of 98.43%, nitrate conversion rate of 94% and NH 3 selectivity of 79.33%. It is found that Ce-doping Cu electrode could tune electronic structure of Cu by generating Cu/Cu 2 O interfacial structure as active phase, which reduces the overpotential of nitrate reduction and improves the NH 3 selectivity of Cu electrodes.
研究领域:
电化学
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材料科学
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环境工程
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催化
✓ 已验证
DOI
高影响因子
ELECTROCHIMICA ACTA
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2019
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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
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材料科学
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纳米技术
✓ 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）