CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Xiaoyu Zhang,Ge Ma,Lingling Shui,Guofu Zhou,Xin Wang
Electrocatalytic nitrate reduction into recyclable ammonium under mild conditions provides an efficient and clean ammonium production strategy and remediation of nitrate-containing wastewater. In this work, we successfully synthesize the Ni 3 N nanoparticles anchored on nitrogen-doped carbon (Ni 3 N/N-C) nanohybrids through simple calcination and acid etching procedures using Ni-dimethylglyoxime complex (Ni-DMG) nanorods as raw material. Physical characterizations confirm that as-synthesized Ni 3 N/N-C nanohybrids have the high specific surface area of 665.7 m 2 g −1 and the ultrafine Ni 3 N nanoparticles (5.3 nm) are dispersed uniformly on the surface of porous nitrogen-doped carbon nanorods. The electrochemical experiments indicate that the combination of nitrogen-doped carbon can greatly improve electroactivity of Ni 3 N nanoparticles for nitrate reduction reaction. Consequently, Ni 3 N/N-C nanohybrids possess high selectivity for ammonium production (89.5%) and high yield rate of ammonium (9.185 mmol h −1 mg Ni3N −1 ) for nitrate electroreduction. Additionally, Ni 3 N/N-C nanohybrids also show excellent long-term stability due to their structural/chemical stability.
研究领域:
环境科学
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材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2019
·
IF 7.723
Xiaozhen Shi,Xin Wen,Shilin Nie,Jie Dong,Jingde Li,Yongqing Shi,Huiling Zhang,Guoyi Bai
Nickel is a highly active catalyst for the semi-hydrogenation of alkynes. However, the low selectivity of the alkene product caused by the over-hydrogenation reaction on Ni has hindered its practical applications. In this work, we report a new nickel nitride (Ni 3 N)-catalyzed semi-hydrogenation of alkynes to the corresponding alkenes. The Ni 3 N nanorods were facilely fabricated via a direct pyrolysis of the solid mixture of nickel acetate tetrahydrate and melamine (Mlm). The Ni 3 N phase in the optimum catalyst (Ni 3 N/NC-6/5-550) is shown to be effective and stable in the semi-hydrogenation of alkynes, with a high yield and good selectivity for alkenes ( Z / E ratios up to >99/1). Both terminal and internal alkynes bearing a broad scope of functional groups are readily converted into alkenes with good chemo- and stereoselectivity. Notably, it was found that the over-hydrogenation can be markedly suppressed even at high conversion of alkyne. Density functional theory (DFT) calculations reveal that the low interaction between the alkene product and the Ni 3 N might plays a critical role in the selectivity enhancement.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
ChemSusChem
·
2024
·
IF 7.5
Hongjing Wang,Wenjie Zhan,Shaojian Jiang,Kai Deng,Ziqiang Wang,You Xu,Hongjie Yu,Liang Wang
Graphical Heterostructure Ni 3 N/WO 3 nanosheet arrays loaded on nickel foam (Ni 3 N/WO 3 /NF) were synthesized by combining cation-exchange with the hydrothermal method and annealing under an ammonia atmosphere (NH 3 ). Ni 3 N/WO 3 nanosheet arrays consist of irregular particles and have abundant active sites due to the heterogeneous interface between Ni 3 N and WO 3 . Ni 3 N/WO 3 /NF was used for efficient electrocatalytic glycerol oxidation coupled to hydrogen production. Glycerol oxidation-assisted water electrolysis has emerged as a cost-effective way of co-producing green hydrogen and HCOOH. Still, preparing highly selective and stable nickel-based metal electrocatalysts remains a challenge. Herein, heterostructure Ni 3 N/WO 3 nanosheet arrays of bifunctional catalysts with large specific surface areas loaded on nickel foam (denoted as Ni 3 N/WO 3 /NF) were synthesized. This catalyst was for glycerol oxidation reaction (GOR) and hydrogen evolution reaction (HER) with excellent catalytic performance, a voltage saving of 267 mV compared to oxygen evolution reaction (OER), and a HER overpotential of 104 mV at 100 mA cm −2 . The cell voltage in the assembled GOR//HER hybrid electrolysis system reaches 100 mA cm −2 at 1.50 V, 296 mV lower than the potential required for overall water splitting. This work demonstrates that replacing GOR with OER using a cost-effective and highly active Ni-based bifunctional electrocatalyst can make hybrid water electrolysis an energy-efficient, sustainable, and green strategy for hydrogen production.
研究领域:
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2020
·
IF 16.683
Peng Zhou,Guangyao Zhai,Xingshuai Lv,Yuanyuan Liu,Zeyan Wang,Peng Wang,Zhaoke Zheng,Hefeng Cheng,Ying Dai,Baibiao Huang
Constructing a suitable coupling interface to improve the performance is of great significance for the development of high-efficient electrocatalysts. Here, we design and synthesize a Ni 3 N-V 2 O 3 composite via nitriding treatment of NiV-LDH precursor, which exhibits excellent electrocatalytic hydrogen evolution reaction (HER) performance including low potential, fast kinetic rate and high stability. Combined with various characterizations and theoretical calculations, the performance promotion mechanism of Ni 3 N-V 2 O 3 is analyzed in depth. It is proved that the confinement effect and interface coupling effect caused by the introduction of V 2 O 3 can greatly increase the catalytic sites, regulate the charge distribution at the interface, optimize the occupancy of the N 2p orbital, and ultimately improve the electrocatalytic HER performance of Ni 3 N. This work provides a new idea and guidance for the design and preparation of high-efficient catalysts in the future.
研究领域:
材料科学
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电化学
✓ 已验证
DOI
高影响因子
CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
·
2022
·Vol. 39
·期 6
·928-932
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IF 2.726
Xu Zhonghang,Wu Yuanyu,Tao Ran,Jin Zhanbin,Fang Xuedong
I n recent years, many effective photocatalysts have been developed to solve the problem of environmental pollution and clean energy shortage. In this paper, non-noble metal cocatalyst Ni 3 N nanoparticles supported Zn 0.5 Cd 0.5 S(ZCS) nanorods(Ni 3 N/ZCS) composites were successfully synthesized by ultrasonic method. The hydrogen production efficiencies of the photocatalysts were tested under visible light, which was found that when the loading of Ni 3 N was 2% of the mass of ZCS, and the Ni 3 N/ZCS composite had the best hydrogen evolution performance, which could reach 70.3 mmol·h −1 ·g −1 . In addition, the quantum efficiency under 420 nm monochromatic light irradiation was 27.2%. Through different characterization analyses, such as X-ray diffraction(XRD), scanning electron microscopy(SEM), and UV-Vis diffuse reflectance spectra(DRS), a possible photocatalytic mechanism was proposed, providing some reference value for non-precious metals as cocatalysts.
研究领域:
材料科学
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环境科学
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能源科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Nano Materials
·
2022
·
IF 6.14
Junrong Zeng,Wenhao Chen,Gaowei Zhang,Liang Yu,Liubiao Zhong,Ya Liu,Sanfei Zhao,Yejun Qiu
Affected by the slow kinetic oxygen evolution reaction (OER), the cell voltage of water splitting is usually beyond 1.5 V, causing high energy consumption to produce hydrogen. Herein, heterostructural Ni3N–NiMoN nanowires supported on carbon cloth (Ni3N–NiMoN/CC) are successfully fabricated, and they can act as bifunctional electrocatalysts, exhibiting a low overpotential of 74 mV at 100 mA cm–2 for hydrogen evolution reaction (HER) and a low potential of 1.39 V at 50 mA cm–2 for 5-hydroxymethylfurfural oxidation reaction (HMFOR), respectively. The HMFOR//HER device constructed by Ni3N–NiMoN/CC achieves a very low cell voltage of ∼1.29 V at 10 mA cm–2, which is 0.32 V lower than that of the OER//HER device. Specially, a value-added product of 2,5-furandicarboxylic acid is obtained. Additionally, density functional theory calculations are carried out. This work provides a promising strategy to further reduce the cell voltage to generate hydrogen by replacing OER with biomass oxidation.
研究领域:
材料科学
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电化学
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可再生能源
✓ 已验证
产品关联
DOI
高影响因子
MICROCHIMICA ACTA
·
2018
·Vol. 185
·期 4
·1-6
·
IF 5.705
Luo Junjun,Zhao Dan,Yang Minghui,Qu Fengli
A glassy carbon electrode was modified with an array of porous Ni 3 N nanosheets (Ni 3 N NA) and studied for its use in non-enzymatic electrochemical detection of glucose. The morphology and structure of the Ni 3 N NA were characterized by scanning electron microscopy and X-ray diffraction. Electrochemical studies demonstrated that the Ni 3 N NA acts as an efficient catalyst for the electro-oxidation of glucose at pH 13, best at a working voltage of 0.55 V (vs. Ag/AgCl). Figures of merit include (a) high sensitivity (39 μA·mM −1 ·cm −2 ), (b) a low limit of detection (0.48 μM), and (c) a linear range that extends from 2 μM to 7.5 mM. The sensor was applied to the determination of glucose levels in human serum, and satisfactory results were obtained.
Nonenzymatic electrochemical glucose sensor based on porous Ni 3 N nanosheet array. The arrow indicates the successive addition of glucose standard solutions.
研究领域:
分析化学
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生物医学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHINESE JOURNAL OF CATALYSIS
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2019
·
IF 4.914
Jianhua Ge,Yujie Liu,Daochuan Jiang,Lei Zhang,Pingwu Du
Photocatalytic H 2 production via water splitting in a noble-metal-free photocatalytic system has attracted much attention in recent years. In this study, noble-metal-free Ni 3 N was used as an active cocatalyst to enhance the activity of g-C 3 N 4 for photocatalytic H 2 production under visible-light irradiation ( λ > 420 nm). The characterization results indicated that Ni 3 N nanoparticles were successfully loaded onto the g-C 3 N 4 , which accelerated the separation and transfer of photogenerated electrons and resulted in enhanced photocatalytic H 2 evolution under visible-light irradiation. The hydrogen evolution rate reached ∼305.4 μmol h −1 g −1 , which is about three times higher than that of pristine g-C 3 N 4 , and the apparent quantum yield (AQY) was ∼0.45% at λ = 420. Furthermore, the Ni 3 N/g-C 3 N 4 photocatalyst showed no obvious decrease in the hydrogen production rate, even after five cycles under visible-light irradiation. Finally, a possible photocatalytic hydrogen evolution mechanism for the Ni 3 N/g-C 3 N 4 system is proposed.
研究领域:
材料科学
·
能源化学
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Weigao Zhong,Qiming Sun,Lin Lv,Yong Han,Zhanghua Hong,Guohua Wang,Xiang Ao,Yuling Zhai,Tao Zhu,Xing Zhu,Hua Wang,Kongzhai Li,Zhishan Li
The exploration and rational design of high-performance, durable, and non-precious-metal bifunctional oxygen electrocatalysts are highly desired for the large-scale application of overall water splitting. Herein, an effective and straightforward coupling approach was developed to fabricate high-performance bifunctional OER/HER electrocatalysts based on core–shell nanostructure comprising a Ni/Ni3N core and a NiFe(OH)x shell. The as-prepared Ni/Ni3N@NiFe(OH)x-4 catalyst exhibited low overpotentials of 57 and 243 mV at 10 mA cm–2 for the HER and OER in 1.0 m KOH, respectively, superior to most bifunctional oxygen electrocatalysts reported so far. Compared to the unmodified Ni/Ni3N, the Ni/Ni3N@NiFe(OH)x-4 catalyst exhibited a 43.3-fold increase in mass activity for the OER and an 8.7-fold increase for the HER, as well as a 29.5-fold increase in intrinsic activity for the OER and a 2.6-fold increase for the HER. When employed as both the cathode and the anode of the electrolyzer for the overall water splitting reaction, its voltage was reduced to 1.58 V at 10 mA cm–2. This surface reconstruction method increased the electrochemically active surface area and enhanced the catalytic activity. Furthermore, in situ Raman spectroscopy revealed that the Fe etching reduced the onset potential for the active phase NiOOH, promoted its formation, and accelerated the reaction kinetics, thereby enhancing the overall electrocatalytic performance of the catalyst.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Energy Chemistry
·
2022
·
IF 13.599
Meng Li,Xiaodong Wu,Kun Liu,Yifan Zhang,Xuechun Jiang,Dongmei Sun,Yawen Tang,Kai Huang,Gengtao Fu
Urea oxidation reaction (UOR), which has favorable thermodynamic energy barriers compared with oxygen evolution reaction (OER), can provide more cost-effective electrons for the renewable energy systems, but is trapped by its sluggish UOR kinetics and intricate reaction intermediates formation/desorption process. Herein, we report a novel and effective electrocatalyst consisting of carbon cloth supported nitrogen vacancies-enriched Ce-doped Ni 3 N hierarchical nanosheets (Ce-Ni 3 N@CC) to optimize the flat-footed UOR kinetics, especially the stiff rate-determine CO 2 desorption step of UOR. Upon the introduction of valance state variable Ce, the resultant nitrogen vacancies enriched Ce-Ni 3 N@CC exhibits an enhanced UOR performance where the operation voltage requires only 1.31 V to deliver the current density of 10 mA cm −2 , which is superior to that of Ni 3 N@CC catalyst (1.36 V) and other counterparts. Density functional theory (DFT) results demonstrate that the incorporation of Ce in Ni 3 N lowers the formation energy of nitrogen vacancies, resulting in rich nitrogen vacancies in Ce-Ni 3 N@CC. Moreover, the nitrogen vacancies together with Ce doping optimize the local charge distribution around Ni sites, and balance the adsorption energy of CO 2 in the rate-determining step (RDS), as well as affect the initial adsorption structure of urea, leading to the superior UOR catalytic performance of Ce-Ni 3 N@CC. When integrating the Ce-Ni 3 N catalyst in UOR//HER and UOR//CO 2 R flow electrolyzer, both of them perform well with low operation voltage and robust long-term stability, proofing that the thermodynamically favorable UOR can act as a suitable substitute anodic reaction compared with that of OER. Our findings here not only provide a novel UOR catalyst but also offer a promising design strategy for the future development of energy-related devices.
研究领域:
材料科学
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电催化
·
可再生能源
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2024
·Vol. 171
·期 5
·056506
·
IF 3.1
Yang Zhou,Kunfeng Zhao,Chenhao Shi,Haojie Ma,Dingwang Yuan,Zhiguo Yi
Electrocatalytic water splitting for hydrogen production is promising, but its practical application is limited by the sluggish kinetics of the anodic oxygen evolution reaction (OER) and the less valuable oxygen by-product. Hence, replacing OER with a thermodynamically favorable methanol oxidation reaction (MOR) and coupling with value-added formate generation on the anode is an energy-saving and effective scheme. In this work, we report a self-supporting bifunctional electrocatalyst MoN/Ni3N/NF, which exhibits excellent hydrogen evolution reaction catalytic activity and stability, requiring overpotentials of only 18 and 68 mV to reach current densities of −10 and −100 mA cm−2, respectively. Moreover, the catalyst's performance minimally deteriorates after long-standing chronopotentiometry measurements (−100 mA cm−2@150 h). When MOR is used instead of OER, the required potential drops by 200 mV to 1.38 V at a current density of 100 mA cm−2 and MoN/Ni3N/NF also demonstrates splendid catalytic stability towards OER and MOR. Finally, a two-electrode system employing MoN/Ni3N/NF as a bifunctional electrocatalyst only requires a cell voltage of 1.40, 1.68 V to achieve current densities of 10 and 100 mA cm−2, respectively. The coupled electrolyzer also exhibits high faradaic efficiency for producing cathodic H2 (100%) and anodic formate (90%).
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 COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Yucheng Dong,Xichun Zhang,Xuyun Wang,Fangfang Liu,Jianwei Ren,Hui Wang,Rongfang Wang
The development of efficient electrocatalysts for large-scale water electrolysis is crucial and challenging. Research efforts towards interface engineering and electronic structure modulation can be leveraged to enhance the electrochemical performance of the developed catalysts. In this work, a surface-engineered Co-Ni 3 N/NF heterostructure electrode was prepared based on Kirkendall effect for high-current water electrolysis. In the experiments, the textural feature and intrinsic activity of the Co-Ni 3 N/NF heterostructure were tuned through cobalt-doping and the creation of structural defects. As a result, the increased surface energy endowed Co-Ni 3 N/NF heterostructure with superhydrophilic and superaerophobic properties. Meanwhile, the contact area of the gas–liquid-solid three phases was optimized. With a large underwater bubble contact angle (CA) of 169°, the electrolyte solution can infiltrate the Co-Ni 3 N/NF electrode within 150 ms. Sequentially, the generated gas bubbles were able to detach at high frequency, which ensured the rapid mass exchange. The performance tests showed that the optimal Co-Ni 3 N/NF electrode sample reached current densities of 100 mA cm −2 and 500 mA cm −2 at the overpotentials of 98 mV and 123 mV, respectively. Benefiting from the reduction of hydrogen embrittlement, the HER performance of the prepared Co-Ni 3 N/NF electrode sample decreased slightly after 100 h durability test, but the overall structure remained well. Those results allowed us to conclude that the prepared Co-Ni 3 N/NF electrocatalyst holds the promises for large-scale water electrolysis in industries. More specifically, this work provided a new perspective that the efficiency of electrocatalysts for large-scale water electrolysis can be enhanced by constructing a heterostructure with good wettability and gas repellency.
研究领域:
材料科学
·
电化学
·
能源催化
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）