JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Linwei Jiang,Yichen Pan,Jiancheng Zhang,Xin Chen,Xinwen Ye,Zhendong Li,Caicai Li,Qingfeng Sun
Replacing the sluggish oxygen evolution reaction (OER) with thermodynamically favorable urea oxidation reaction (UOR) is an appealing tactic in the energy-saving water splitting system. Herein, by a facile composite electrodeposition method, an electrocatalyst with Mo particles anchored on the Ni-P matrix (Mo/Ni-P) was fabricated and utilized for urea-assisted water electrolysis of hydrogen production. As expected, the urea-involved electrolytic cell with the as-obtained Mo/Ni-P served as both the anode and cathode merely needs a voltage of 1.55 V to sustain a current density of 50 mA cm −2 (0.16 V less than that of the conventional water splitting at 50 mA cm −2 ) and can maintain the stability for 12 h. Additionally, the solar-driven urea-assisted water electrolysis system was constructed under lab conditions and solar-hydrogen-electricity energy conversion processes were also simulated. Moreover, it was demonstrated that tungsten (W) particles can also serve as an accelerant for promotion both the hydrogen evolution reaction (HER) and UOR activity of pristine Ni-P. This work will present a facile method for rational integration of metal particles with Ni-P layer for highly efficient electrocatalysts applied in economic production of H 2 .
研究领域:
能源材料
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Na Wu,Xiaoqiang Du
One of the most attractive means for mitigation of environmental pollution is to produce hydrogen by electrocatalytic urea splitting. In the paper, the heterogeneous interfacial rich N–CuCo 2 S 4 @Ni 3 S 2 material was in situ synthesized on nickel foam through a typical hydrothermal and sulfuration process. This N–CuCo 2 S 4 @Ni 3 S 2 electrode displays excellent urea oxidation performance (potential of 1.38 V@50 mA cm −2 ), which is one of the best reactivity reported so far. Experimental results show that the superior catalytic activity is attributed to the rapid charge transfer, more reaction center exposed and superior electrical conductivity . Density functional theory shows that this Ni 3 S 2 material accelerates the reaction rate in the catalytic process, the introduction of this N–CuCo 2 S 4 material improves the conductivity of the material, and the synergistic catalysis of the N–CuCo 2 S 4 and Ni 3 S 2 makes this N–CuCo 2 S 4 @Ni 3 S 2 material exhibit superior urea oxidation activity. Notably, long-term tests have shown a decrease in catalytic activity, which suggests that the surface of the sulfide is in situ generated to oxides or hydroxides, which are truly active species. This work provides a new idea for the development of efficient and stable urea oxidation catalysts for sulfides.
研究领域:
材料科学
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环境科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
MOLECULES
·
2023
·Vol. 28
·期 20
·7147
·
IF 4.6
Xiafei Gao,Mengyue Gao,Xueping Yu,Xiaoyong Jin,Gang Ni,Juan Peng
The very slow anodic oxygen evolution reaction (OER) greatly limits the development of large-scale hydrogen production via water electrolysis. By replacing OER with an easier urea oxidation reaction (UOR), developing an HER/UOR coupling electrolysis system for hydrogen production could save a significant amount of energy and money. An Al-doped cobalt ferrocyanide (Al-Co2Fe(CN)6) nanocube array was in situ grown on nickel foam (Al-Co2Fe(CN)6/NF). Due to the unique nanocube array structure and regulated electronic structure of Al-Co2Fe(CN)6, the as-prepared Al-Co2Fe(CN)6/NF electrode exhibited outstanding catalytic activities and long-term stability to both UOR and HER. The Al-Co2Fe(CN)6/NF electrode needed potentials of 0.169 V and 1.118 V (vs. a reversible hydrogen electrode) to drive 10 mA cm−2for HER and UOR, respectively, in alkaline conditions. Applying the Al-Co2Fe(CN)6/NF to a whole-urea electrolysis system, 10 mA cm−2was achieved at a cell voltage of 1.357 V, which saved 11.2% electricity energy compared to that of traditional water splitting. Density functional theory calculations demonstrated that the boosted UOR activity comes from Co sites with Al-doped electronic environments. This promoted and balanced the adsorption/desorption of the main intermediates in the UOR process. This work indicates that Co-based materials as efficient catalysts have great prospects for application in urea electrolysis systems and are expected to achieve low-cost and energy-saving H2production.Keywords:hydrogen;urea oxidation;electronic structure;energy-saving;cobalt ferrocyanide
研究领域:
电化学
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材料科学
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能源工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Materials Chemistry Frontiers
·
2024
·
IF 6
Xin Fu,Bo Pu,Li Pan,Ruiqi Ming,Qian Lv,Xiaobo Chen,Lihong Tian
Urea oxidation reaction (UOR) is a promising substitution for the oxygen evolution reaction (OER) on anode for highly efficient H2 production. However, the sluggish kinetics and high oxidation potential of NiII → NiIII severely limit the activity of Ni-based catalysts in the electrochemical UOR. Herein, composition regulation was adopted to enhance the electrocatalytic activity of a nickel-benzene dicarboxylate framework (Ni-BDC MOF)-derived electrode towards urea oxidation. In 1 M KOH with 0.33 M urea solution, the derived amorphous tri-metallic hydroxide layer on the surface of the NiMnCo MOF, induced by electro-activation, exhibited a low onset potential and a steeply rising current density with increasing applied potential. It achieved a benchmark current density of 10/100 mA cm−2 at an anode potential of 1.28/1.33 V vs. RHE, respectively. In particular, a 500 mA cm−2 current density was reached at an impressively low potential of 1.41 V vs. RHE. This exceptional performance is ascribed to the fact that the open framework provides a large electrochemical active surface, while the multicomponent synergy decreases the NiII → NiIII oxidation potential, enhances electron transfer and promotes the UOR kinetics. This study suggests that rational composition regulation is a promising approach to improving the performance of Ni-based MOF materials towards electrocatalytic urea oxidation.
研究领域:
材料科学
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电化学
·
催化
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF APPLIED ELECTROCHEMISTRY
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2020
·Vol. 50
·期 11
·1091-1099
·
IF 2.384
Fa Dejuan,Miao Yuqing
Abstract The NiHPO 4 –Ni(OH) 2 nanowire-assembled bouquets were easily synthesized. Scanning electron microscopy and transmission electron microscopy show the NiHPO 4 –Ni(OH) 2 bouquets form through the organization of nanowires which arrange with certain direction. The electrocatalytic activities of NiHPO 4 –Ni(OH) 2 –GCE towards the oxidation of methanol and urea were studied in NaOH. The nanowire-assembled bouquets were modified on the surface of the glassy carbon electrode, leading to the increase on the surface area of the electrode, which in turn enhanced the current density and electrocatalytic performance for the oxidation of methanol and urea. It shows the potential applications for the utilization of these energy molecules. Graphic abstract
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Pengyang Jiang,Baoxin Ge,Jiaqing Liu,Caijin Huang,Xue Feng Lu
Urea oxidation reaction (UOR) kinetics is severely limited by suboptimal intermediate adsorption, which can be significantly improved by modulating catalyst spin configurations. Herein, we report an effective strategy for reforming the Ru spin configuration in pyrochlore oxide Y 2 Ru 2 O 7 (YRO) to enhance UOR performance through gradient orbital coupling. By partially substituting Y with Sm, we precisely regulate the electronic structure of candidate Y 1.9 Sm 0.1 Ru 2 O 7 (YRO-Sm), transforming Ru spin configuration from the low spin to the high spin (HS) configuration. The HS configuration endows YRO-Sm with excellent UOR activity (1.43 V at j = 100 mA cm −2 ) and robust stability. Theoretical analysis reveals that Sm substitution leads to a significant Sm(4 f)–O(2p)–Ru(4d) orbital electron coupling effect. The highly degenerate 4 f orbitals of Sm enhance Ru–O covalency and Ru electron localization in YRO-Sm, facilitating *COO intermediate dissociation and thereby lowering the energy barrier for UOR. The practical potential of YRO-Sm was further demonstrated through its successful integration into both a hybrid water electrolyzer for energy-saving hydrogen production and a urea-assisted zinc–air battery. This work demonstrates a promising pathway for developing high-performance pyrochlore catalysts via spin state engineering for sustainable energy conversion applications.
研究领域:
催化
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材料科学
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电化学
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能量转换
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无机化学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Youwei Cheng,Lian Zhu,Yaqiong Gong
Metal-organic frameworks (MOFs) are widely recognized as precursors or sacrificial templates for the synthesis of target catalysts on account of their high porosity and high active surface area . Elemental doping strategy is considered as an effective method for the synthesis of efficient and stable catalysts for electrolytic water. Therefore, in this paper, Ce-doped Ni(OH) 2 nanoparticles and Ni-MOF nanosheets composites were synthesized by electrodeposition using Ni-MOF as precursor. Catalyst Ce–Ni(OH) 2 @Ni-MOF/NF displays excellent OER performance, requiring only 193 mV and 279 mV overpotentials to realize current densities of 10 mA cm −2 and 100 mA cm −2 , respectively, while the UOR performance was very remarkable, only a potential of 1.28 V was demanded to reach a current density of 10 mA cm −2 . In addition, no obvious change in the overpotential was noticed during the stability test of 16 h, indicating good stability of Ce–Ni(OH) 2 @Ni-MOF/NF. This study provides a meaningful reference for the design of an efficient and stable environmental friendly electrocatalyst .
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Jing Wang,Min Wang,Zhenjiang Lu,Jing Xie,Jianguo Huang,Jindou Hu,Yali Cao
The inefficient Ni/Fe ion utilization and poor electrical conductivity of nickel-iron layered double hydroxide (NiFe-LDH) restricts to its development in electrocatalytic oxygen evolution reaction/urea oxidation reaction (OER/UOR). Herein, self-supported Hf-doped NiFe-LDH nanosheet arrays were successfully prepared on nickel foam (Hf-NiFe-LDH/NF) via a one-step solvothermal approach for the first time, in which the introduced high-valent Hf 4+ altered the structure of electrons and chemical environment of the atoms and promoted the production of more active sites, thus realizing the fast kinetics of electron transfer on the layer. Meanwhile, the doped metal Hf ions increased the electric conduction and recycling stability of the catalyst. Astoundingly, the overpotential of Hf-NiFe-LDH/NF is barely 258 mV at a current density of 100 mA cm −2 , which is 61 mV lower than that of NiFe-LDH/NF, as well as outstanding stability for over 90 h during the OER. Similarly, the potential is only 1.37 V at 100 mA cm −2 during the UOR, 118 mV less was than at OER. Notably, Hf-NiFe-LDH/NF electrocatalyst exceeds the most previously reported electrocatalysts in terms of performance. This study highlights the benefits of Hf doping strategy in electrocatalytic OER/UOR and presents a promising new type of catalyst for future research.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2025
·
IF 7.9
Man Zhao,Zimei Fu,Wei Wen,Yuhong Chang,Wenxiang Wang,Meng Bai,Xiaoli Li,Li Zhang,Junming Zhang,He Xiao,Jianfeng Jia
Up to now, nickel-based materials have been considered as the most promising catalysts for urea oxidation reaction (UOR). However, the inevitable self-oxidation from Ni 2+ to Ni 3+ severely limited their activity during UOR. To trigger the UOR occurred before self-oxidation of Ni species by altering reaction pathways, here synergistic dual-site of Cu 3 P-NiO x on black phosphorus (BP) nanosheets is constructed by a facile self-designed electrosynthesis method, where exfoliation of bulky BP into nanosheets and formation of multivalent Ni or Cu precursor are both obtained during electrosynthesis process. The best Cu 3 P-NiO x /BP shows the potential of 1.378 V under light irradiation at 10 mA cm −2 (without IR compensation), 187 mV lower than that in oxygen evolution reaction. This UOR activity of Cu 3 P-NiO x /BP is superior to Cu 3 P/BP or NiO x /BP, which is attributed to synergistic dual-site constructure of Cu 3 P-NiO x . In-situ and ex-situ characterizations suggest that in-situ generated Cu 3 P promotes adsorption and activation of urea molecules, and takes synergistic effect with NiO x , which makes urea oxidation undergoes a direct complete oxidation process. Moreover, with application of light illumination, excited photoelectrocatalytic effect by Cu 3 P further greatly enhances the activity for UOR. This study provides insights to the designing principles for optimizing reaction pathways toward small nucleophile molecule oxidation and effective strategies to develop efficient UOR photoelectrocatalysts.
研究领域:
材料科学
·
电化学
·
催化反应
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2025
·
IF 17.7
Jiaxin Li,Yan Lv,Xueyan Wu,Xinyu Guo,Zhuojun Yang,Jixi Guo,Tianhua Zhou,Dianzeng Jia
To address the high cost and limited electrochemical endurance of Pt-based electrocatalysts, the appropriate introduction of transition metal-based compounds as supports to disperse and anchor Pt species offers a promising approach for improving catalytic efficiency. In this study, sub-1 nm Pt nanoclusters were uniformly confined on NiO supports with a hierarchical nanotube/nanosheet structure (Pt/NiO/NF) through a combination of spatial domain confinement and annealing. The resulting catalyst exhibited excellent electrocatalytic activity and stability for hydrogen evolution (HER) and urea oxidation reactions (UOR) under alkaline conditions. Structural characterization and density functional theory calculations demonstrated that sub-1 nm Pt nanoclusters were immobilized on the NiO supports by Pt–O–Ni bonds at the interface. The strong metal-support interaction induced massive charge redistribution around the heterointerface, leading to the formation of multiple active sites. The Pt/NiO/NF catalyst only required an overpotential of 12 and 136 mV to actuate current densities of 10 and 100 mA cm −2 for the HER, respectively, and maintained a voltage retention of 96% for 260 h of continuous operation at a current density of 500 mA cm −2 . Notably, in energy-efficient hydrogen production systems coupled with the HER and UOR, the catalyst required cell voltages of 1.37 and 1.53 V to drive current densities of 10 and 50 mA cm −2 , respectively—approximately 300 mV lower than conventional water electrolysis systems. This study presents a novel pathway for designing highly efficient and robust sub-nanometer metal cluster catalysts.
研究领域:
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2021
·
IF 5.706
Guoqiang Liu,Cheng Huang,Zeheng Yang,Jianhui Su,Weixin Zhang
Water electrolysis has been widely considered as a promising technique for generating hydrogen. However, oxygen evolution reaction (OER) as a sluggish anodic reaction, usually suffers from high overpotential, which greatly impedes the efficiency of hydrogen generation. Herein, we report an ultrathin NiMn-LDH/CFC growth on commercial carbon fiber cloth (U-NiMn-LDH/CFC) substrate through a facile hydrothermal method. The U-NiMn-LDH/CFC can be successfully used to assemble an energy-saving water splitting system via integrating anodic urea oxidation reaction (UOR) and hydrogen evolution reaction (HER). The as-prepared U-NiMn-LDH/CFC nanosheets with ultrathin structure exhibit reliable electrocatalytic activities toward UOR (1.351 V vs. RHE@20 mA cm −2 ) and HER (169 mV@10 mA cm −2 ). A two-electrode water splitting cell is further constructed and delivers almost 210 mV lower oxidation potential at 10 mA cm −2 with containing (1.0 M KOH) 0.5 M urea in comparison to that in pure overall water splitting. Furthermore, the above two-electrode system shows excellent electrolysis stability.
研究领域:
材料科学
·
能源化学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2023
·
IF 6.6
Sirong Li,Yipeng Zhang,Xin Yu,Zhenlong Wang,Guofei Zhang,Zhengyi Zhao,Zhiyong Yan,Xuechun Xiao
An environmentally friendly method of producing hydrogen is electrocatalytic water splitting, but the high theoretical potential of the anode's OER (1.23 V vs. RHE) restricts the efficiency of hydrogen production . Therefore, using the urea oxidation reaction (UOR, theoretical potential of 0.37 V vs. RHE) in place of the OER can significantly increase the efficiency of hydrogen production. Here, we grow the hydroxide layer of Ni-Co-Fe directly on NF by one-step electrodeposition and obtain the best catalyst by regulating the elemental ratio of Co and Fe. Through tests, it is found that NiCoFe(OH) x /NF(Co: Fe=3: 1) exhibits the best electrocatalytic performance, and the required potential is only 1.24 and 1.30 V when the current density reaches 10 and 50 mA cm −2 in the UOR process, which is 170 and 140 mV lower than the OER overpotential under the same conditions, showing a more advantageous anodic catalytic effect. At the same time, integral water decomposition in an electrolyte of 1 M KOH adds with 0.5 M urea also shows more favorable catalytic activity and stability. The NiCoFe(OH) x /NF(Co: Fe=3: 1) plays an important role in improving the efficiency of hydrogen production by water splitting through simple electrodeposition, and has sustainable development prospects.
研究领域:
材料科学
·
电化学
✓ 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）