INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2019
·
IF 4.084
Qilu Yao,Meng He,Xiaoling Hong,Xinyu Chen,Gang Feng,Zhang-Hui Lu
Hydrazine borane (N 2 H 4 BH 3 , 15.4 wt%) and hydrous hydrazine (N 2 H 4 ·H 2 O, 8 wt%) are promising chemical hydrogen storage materials that have attracted much attention in recent years due to their high gravimetric hydrogen capacities. The selective and rapid catalytic dehydrogenation of N 2 H 4 BH 3 and N 2 H 4 ·H 2 O is the key to the potential use of the abovementioned materials in hydrogen applications. In this study, a series of Rh-MoO x nanoparticles (NPs) with various metal compositions have been successfully prepared via a simple one-step chemical reduction approach in the absence of a surfactant/support at room temperature . The obtained surfactant/support-free Rh-MoO x NPs exhibit good dispersibility and small particle size. Among all of the as-prepared Rh-MoO x NPs, the optimized Rh-MoO x catalysts with a molar ratio of 1:1 show the highest catalytic properties with 100% H 2 selectivity for hydrogen evolution from aqueous N 2 H 4 BH 3 and N 2 H 4 ·H 2 O solutions at 323 K under alkaline conditions. The turnover frequency (TOF) values of Rh 0.5 (MoO x ) 0.5 NPs are 2000 and 750 h −1 for hydrogen evolution from N 2 H 4 BH 3 and N 2 H 4 ·H 2 O , respectively, which are among the highest values ever reported for Rh-based catalysts. The superior catalytic performances could be attributed to the small particles size, low crystallinity , modified electronic structure, and strong basic sites of Rh NPs induced by the MoO x dopant . The highly rapid and selective Rh-MoO x catalyst may further encourage the deployment and application of N 2 H 4 BH 3 and N 2 H 4 ·H 2 O as safe and convenient sources of hydrogen for fuel cells.
研究领域:
化学工程
·
材料科学
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2016
·
IF 3.014
Jianmin Chen,Zhang-Hui Lu,Wei Huang,Zhibing Kang,Xiangshu Chen
NiPt nanoparticles (NPs) supported on graphene nanosheets were successfully synthesized via a galvanic replacement approach at room temperature with precursor Ni NPs as a sacrificial template. The as-synthesized NiPt/graphene catalysts were characterized by inductively coupled plasma, X-ray diffraction, transmission electron microscopy , high-angle annular dark field scanning transmission electron microscopy , X-photoelectron spectroscopy, and BET surface area measurement, and used as catalysts for H 2 production from hydrazine and hydrazine borane. The characterization data showed that NiPt NPs with a small size of around 3.5 nm were dispersed on the graphene nanosheets. The as-synthesized NiPt/graphene exhibited high activity and 100% hydrogen selectivity toward the conversion of hydrazine or hydrazine borane to hydrogen. The turnover frequency ( TOF ) values of Ni 0.58 Pt 0.42 /graphene reached 434 h −1 at 30 °C and 846 h −1 at 50 °C for the decomposition of hydrazine, respectively, which are higher than those of most of the reported catalysts. In particular, a high TOF value of 2303 h −1 at 50 °C was obtained for dehydrogenation of hydrazine borane, which is among the highest for all the catalysts reported to date. The as-synthesized Ni 0.58 Pt 0.42 /graphene exhibited satisfactory durability for hydrogen evolution from hydrazine and hydrazine borane. This excellent catalytic performance could be attributed to the strong interaction of NiPt NPs and graphene, the small size and high dispersion of NiPt NPs, and NaOH promotion. The development of high catalytic activity catalysts is a promising step towards the application of hydrazine and hydrazine borane as hydrogen storage material .
研究领域:
材料科学
·
化学工程
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Haiyun Ma,Lixia Yang,Chaoqun Yao,Shuainan Zhao,Fengjun Jiao,Guangsheng Luo,Guangwen Chen
The addition reaction of ethylene oxide (EO) and hydrazine hydrate (N 2 H 4 ·H 2 O) to β-hydroxyethyl hydrazine (HEH) is an important process for the synthesis of hydrazine-derived monopropellant in the aerospace industry. Due to the complexity of this reaction mechanism, it is difficult to reduce the formation of byproducts and efficiently obtain pure HEH. Hence it is necessary to investigate process behavior and establish kinetic network for further optimization. Here a continuous microflow system was developed to systematically investigate the synthesis of HEH under high pressure in the liquid–liquid form. A simple and effective pre-column derivatization method was applied to characterize and quantify the product. Subsequently, a thorough optimization of parameters, including N 2 H 4 ·H 2 O concentration, molar ratio (N 2 H 4 ·H 2 O/EO), temperature and reaction time, was conducted. Additionally, response surface methodology was employed to optimize the reaction conditions, illuminating the intricate interactions among the specified variables and achieving a high HEH yield of 96.97 %. Finally, a kinetic model was established, and the activation energies for the main reaction and side reaction were measured to be 38.31 kJ·mol −1 and 44.94 kJ·mol −1 , respectively. This kinetic model can enable the accurate determination of kinetic parameters and provide guidance for the process intensification of this EO addition reaction.
研究领域:
化学工程
·
航空航天工业
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Wenxin Wang,Jiangjiang Zhang,Jinsheng Rong,Lanli Chen,Shiqiang Cui
Reducing the size of catalysts and tuning their electronic structure and interfacial properties are key to enhancing catalytic performance. Herein, a series of quantum-sized Co-based nanodot composites, including Co 3 O 4 /C, CoS 2 /C, CoN/C, and CoP/C, were synthesized using chemical vapor deposition (CVD) methods. By means of experimental measurement and theoretical calculation, CoP/C exhibited more robust electrochemical response than other Co-based compounds in electrochemical oxidation of N 2 H 4 (HzOR) and hydrogen evolution reaction (HER). The catalytic activities of CoP/C can be further enhanced by introducing Co vacancies on the surface of CoP/C (labeled as Co 1−x P/C). The results demonstrated that Co 1−x P/C not only exhibited notable electrochemical responses at an ultra-low N 2 H 4 concentration of 0.67 μM, showcasing its potential for ultra-sensitive N 2 H 4 detection but also realized HzOR instead of the oxygen evolution reaction (OER) half-reaction, thereby lowering the overpotential to 2.0 mV at 10.0 mA cm −2 . Finally, a Zn-hydrazine (Zn-Hz) battery was fabricated as a promising energy conversion device, showing the exceptional practical value of Co 1−x P/C.
研究领域:
材料科学
·
电化学
·
能源转换
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Inorganic Chemistry Frontiers
·
2019
·Vol. 6
·期 9
·2271-2278
·
IF 5.934
Xiaoling Hong,Qilu Yao,Meiling Huang,Hongxia Du,Zhang-Hui Lu
Recently, the utilization of hydrazine borane (N2H4BH3) and hydrous hydrazine (N2H4·H2O) as promising hydrogen carriers has received increasing research interest. In this work, NiIr alloy nanoparticles (NPs) immobilized on lanthanum oxy-carbonate (NiIr/La2O2CO3) have been successfully synthesized through a sodium–hydroxide-assisted reduction approach at room temperature. It was found that ultrafine NiIr NPs with an average size of around 2.3 nm were effectively and highly dispersed on La2O2CO3. NiIr/La2O2CO3 nanocomposites (NCs) prepared with the assistance of NaOH showed much higher catalytic activity and H2 selectivity toward the N2H4BH3 dehydrogenation reaction as compared to those of NiIr/La2O2CO3–N prepared without addition of NaOH. Among all of the tested samples, the optimized Ni0.75Ir0.25/La2O2CO3 NCs exhibited the highest catalytic performance with 100% hydrogen selectivity for hydrogen generation from an aqueous solution of N2H4BH3. The total turnover frequency (TOF) of Ni0.75Ir0.25/La2O2CO3 NCs for this dehydrogenation reaction was found to be 1250 h−1 at 323 K, which is among the highest values ever reported. Additionally, this catalyst also exhibited a remarkable catalytic performance for efficient and complete decomposition of N2H4·H2O. This excellent catalytic performance could be attributed to the high dispersion of metal NPs and the strong interaction between the metal and support as well as the promotion effect of NaOH.
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2017
·
IF 3.133
Kun Yang,Kangkang Yang,Shiliang Zhang,Yan Luo,Qilu Yao,Zhang-Hui Lu
Trimetallic NiFePd nanoparticles (NPs) anchored on metal-organic framework (MOF) MIL-101 have been facilely prepared via a simple impregnation method. The as-prepared NiFePd/MIL-101 catalysts have been characterized by powder X-ray diffraction (XRD), scanning electron microscope (SEM), transmission electron microscope (TEM) equipped with energy dispersed X-ray detector (EDX) and selected area electron diffraction (SAED), inductively coupled plasma-atomic emission spectroscopy (ICP-AES), N 2 adsorption/desorption isotherms and X-ray photoelectron spectroscopy (XPS) techniques. And the as-synthesized catalysts have been applied for hydrogen generation from aqueous alkaline solution of hydrazine borane (HB, N 2 H 4 BH 3 ). Compared to the pure Ni 0.36 Fe 0.24 Pd 0.4 NPs, MIL-101 supported mono- and bi-metallic counterparts, the Ni 0.36 Fe 0.24 Pd 0.4 /MIL-101 catalyst exhibits much higher catalytic performance for complete conversion of N 2 H 4 BH 3 to H 2 with 100% selectivity at 323 K. The turnover frequency ( TOF ) value for the dehydrogenation of N 2 H 4 BH 3 in the presence of Ni 0.36 Fe 0.24 Pd 0.4 /MIL-101 catalyst reaches 60 h −1 . Remarkably, the Ni 0.36 Fe 0.24 Pd 0.4 /MIL-101 catalyst also shows high catalytic activity and 100% selectivity towards hydrogen generation from hydrous hydrazine (N 2 H 4 ·H 2 O) at 323 K with a TOF value of 40.8 h −1 . In addition, the durability tests exhibit that the Ni 0.36 Fe 0.24 Pd 0.4 /MIL-101 catalyst is still highly active in the complete dehydrogenation of N 2 H 4 BH 3 and decomposition of N 2 H 4 ·H 2 O with 100% hydrogen selectivity even after five recycles.
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2020
·
IF 4.65
Hongtao Zou,Shiliang Zhang,Xiaoling Hong,Qilu Yao,Yan Luo,Zhang-Hui Lu
As an ideal hydrogen supplier in liquid phase, hydrous hydrazine has gained a lot of attention for safe and efficient storage as well as transportation of hydrogen. Herein, a low Pt-containing Ni–Pt bimetallic catalyst immobilized on novel MIL-101/rGO composite has been prepared by a facile impregnation-reduction approach. Unexpectedly, the resultant Ni 0.9 Pt 0.1 /MIL-101/rGO catalyst exhibits optimal catalytic performance and 100% H 2 selectivity for hydrogen evolution from hydrous hydrazine under alkaline conditions at 323 K, giving a turnover frequency (TOF) value of 960.0 h −1 , which is a relatively higher value ever reported heterogeneous catalysts. Even at room temperature, Ni 0.9 Pt 0.1 /MIL-101/rGO catalyst shows excellent catalytic activity for dehydrogenation of hydrazine as well as hydrazine borane. In addition, the Ni 0.9 Pt 0.1 /MIL-101/rGO catalyst also exhibits excellent durability. Even after eight recycles, the catalytic activity is no significant decrease, and the H 2 selectivity still remains 100%.
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
高影响因子
Inorganic Chemistry Frontiers
·
2017
·Vol. 5
·期 2
·370-377
·
IF 4.036
Zhujun Zhang,Shiliang Zhang,Qilu Yao,Gang Feng,Meihua Zhu,Zhang-Hui Lu
Metal–organic framework (MOF) immobilized Rh–Ni alloy nanoparticles (NPs) with a mean size of 2.8 nm have been facilely and successfully fabricated via a reduction rate controlled method. Bimetallic NP/MOF composites with uniform tiny RhNi alloy NPs immobilized on MOFs, high surface areas (1970 m2 g−1), and accessible porous structure have been obtained. The resulting RhNi/MOF catalysts show high catalytic activity and robust durability for complete H2 evolution from hydrazine borane (N2H4BH3) and hydrous hydrazine (N2H4·H2O). The optimized Rh0.8Ni0.2/MIL-101 catalyst exhibits excellent catalytic performance for the dehydrogenation of N2H4BH3 and N2H4·H2O in aqueous solution with 100% conversion and hydrogen selectivity, high total turnover frequencies (TOF), up to 1200 and 428.6 mol(H2) mol(Rh+Ni)−1 h−1, respectively, the highest over Rh-based catalysts. The high activity and prominent durability of Rh0.8Ni0.2/MIL-101 are highly dependent on the features of the MOF immobilized tiny RhNi alloy NPs, the strong interaction between the MOF crystal and RhNi alloy NPs, the optimized surface and electronic structure of RhNi alloy with an atomic ratio of 8 : 2, and the accessible open porous structure for free mass transfer.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2020
·
IF 4.939
Hui Wang,Jieting Ding,Palanisamy Kannan,Shan Ji
Developing an efficient low-cost and high performance electrocatalyst for electro-oxidation of hydrazine is one of the key challenges in the prospect of direct hydrazine fuel cell (DHFC) application. In this work, a series of nitrogen doped three-dimensional porous Co 3 O 4 /carbon nanosheet network catalysts are synthesized (Co-NPC NNs- x ), and simultaneously characterized by using scanning electron microscopy (SEM), transmission electron microscopy (TEM), x-ray diffraction (XRD), x-ray photoelectron spectroscopy (XPS), and electrochemical methods . Among them, Co-NPC NNs-2 is found to be a potential electrocatalyst towards highly efficient electro-oxidation of hydrazine. The electrochemical results clearly display that Co-NPC NNs-2 catalyst shows enhanced electro-oxidation (low-onset oxidation potential, higher catalytic current response), and higher cycling stability (catalytic response retained even after 120 successive cycles) toward hydrazine when compared to Co-NPC NNs-1, Co-NPC NNs-3, and NPC NNs catalysts modified electrodes . The existence of large active surface area, higher active catalytic sites, and synergetic activity between NPC NNs and Co 3 O 4 NPs (Co-NPC NNs-2) are vital factors mainly attributes to the superior electro-oxidation response of hydrazine. Further, the Co-NPC NNs-2 catalyst demonstrated longer durability towards the electro-oxidation of hydrazine, which is highly comparable with commercially available Pt/C catalyst. Such an efficient low-cost electrocatalyst nanomaterial can enable the use of hydrazine as a promising energy carrier for DHFCs, which increases its practicality for upcoming energy storage and conversion applications.
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
RSC Advances
·
2019
·Vol. 9
·期 12
·6717-6723
·
IF 3.049
Xiuli Dong,Jiayuan Tang,Yan Ren,Xiangming Chen
A novel fluorescence labeling reagent N-acetylhydrazine acridone (AHAD) was designed and synthesized. A highly sensitive high performance liquid chromatography (HPLC) method coupled with fluorescence detection to determine benzaldehyde after derivatization with AHAD was developed. Optimum derivatization was obtained at 40 °C for 30 min with trichloroacetic acid as catalyst. Benzaldehyde derivative was separated on a reversed-phase SB-C18 column in conjunction with a gradient elution and detected by fluorescence detection at excitation and emission wavelengths of 371 nm and 421 nm. The established method exhibited excellent linearity over the injected amount of benzaldehyde of 0.003 to 5 nmol mL−1. The method was successfully applied to the determination of serum semicarbazide-sensitive amine oxidase (SSAO) activity in humans. SSAO is a significant biomarker because serum SSAO activity is elevated in patients with Alzheimer's disease, vascular disorders, heart disease and diabetes mellitus. It was demonstrated that the SSAO activity of the hyperglycemic group (60 ± 4 nmol mL−1 h−1) was significantly higher than that of normal blood sugar group (44 ± 4 nmol mL−1 h−1) with P < 0.05.
研究领域:
分析化学
·
医学
·
生物化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INORGANIC CHEMISTRY
·
2017
·
IF 4.857
Zhujun Zhang,Shiliang Zhang,Qilu Yao,Xiangshu Chen,Zhang-Hui Lu
The catalytic dehydrogenation of hydrazine borane (N2H4BH3) and hydrous hydrazine (N2H4·H2O) for H2 evolution is considered as two of the pivotal reactions for the implementation of the hydrogen-based economy. A reduction rate controlled strategy is successfully applied for the encapsulating of uniform tiny NiPt alloy nanoclusters within the opening porous channels of MOFs in this work. The resultant Ni0.9Pt0.1/MOF core–shell composite with a low Pt content exerted exceedingly high activity and durability for complete H2 evolution (100% hydrogen selectivity) from alkaline N2H4BH3 and N2H4·H2O solution. The features of small NiPt alloy NPs, strong synergistic effect between NiPt alloy NPs and the MOF, and open pore structure for freely mass transfer made NiPt/MIL-101 an excellent catalyst for highly efficient H2 evolution from N2H4BH3 or N2H4·H2O.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Energy & Environmental Science
·
2022
·Vol. 15
·期 8
·3246-3256
·
IF 39.714
Qian Liu,Xiaobin Liao,Yuanhao Tang,Jianghao Wang,Xiangzhou Lv,Xuelei Pan,Ruihu Lu,Yan Zhao,Xin-Yao Yu,Hao Bin Wu
Exploring advanced electrocatalysts for the hydrazine oxidation reaction (HzOR) could expedite the applications of direct hydrazine fuel cells (DHzFCs) for zero-carbon economics. Herein, we report a remarkable HzOR electrocatalyst based on low-coordinated Co arrays supported on Cu foam (p-Co/CF). The low-coordinated Co arrays were synthesized by the reduction of the Co(OH)F precursor with H2 plasma to induce numerous few-atom vacancies, producing low-coordinated surface Co atoms as catalytic active sites. The as-prepared p-Co/CF electrode exhibits a low onset potential of −0.15 V (vs. RHE) and a small Tafel slope of 8.83 mV dec−1 in 0.05 M N2H4/1 M KOH electrolyte, which are superior to those of most reported electrocatalysts toward the HzOR. Density functional theory (DFT) calculations have been employed to elucidate the HzOR process on metallic Co catalysts, suggesting that the improved catalytic activity would be attributed to the weakened adsorption of N2H3* on low-coordinated Co sites. Benefited by the superior catalytic activity of p-Co/CF, a prototype DHzFC has been demonstrated to deliver a high open circuit voltage of 1.1 V and a maximal power density of 186 mW cm−2 at ambient temperatures. This work provides guidance for designing high-performance non-noble metal electrocatalysts toward viable direct hydrazine fuel cells.
研究领域:
材料科学
·
电化学
·
能源科学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）