RENEWABLE ENERGY
·
2019
·
IF 5.439
Qilu Yao,Kangkang Yang,Wendan Nie,Yaxing Li,Zhang-Hui Lu
Hydrazine borane (N 2 H 4 BH 3 ) has been considered as a promising chemical hydrogen storage material in recent years for its high hydrogen content (15.4 wt%), easy preparing, and good stability. Designing highly efficient and selective catalysts for realizing the hydrogen evolution from N 2 H 4 BH 3 is highly attractive but still remains challenging. In this work, NiPd nanoparticles (NPs) modified with MoO x have been readily synthesized via a co-reduction route at room temperature and served as highly efficient catalysts toward hydrogen generation from N 2 H 4 BH 3 in aqueous solution. Compared to the pure Ni 0.6 Pd 0.4 NPs, the obtained Ni 0.6 Pd 0.4 -MoO x catalyst exhibits much higher catalytic performances in dehydrogenation of N 2 H 4 BH 3 at 323 K, providing a total turnover frequency (TOF) value of 405 h −1 and almost 100% hydrogen selectivity. The improved catalytic activity of NiPd-MoO x catalyst may be attributed to the small particles size and increased electron density of NiPd as well as the strong basic sites of NiPd NPs induced by the MoO x dopant . The facile synthesis of high-performance and cost-effective of metal NPs catalysts is of great significance for the development of N 2 H 4 BH 3 as a promising 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
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2016
·
IF 3.205
Kangkang Yang,Qilu Yao,Wei Huang,Xiangshu Chen,Zhang-Hui Lu
In this work, a series of Ni 1-x M x (M = Cr, Mo, W) nanoparticles (NPs) have been successfully synthesized via a simple surfactant-aided co-reduction method and employed as highly efficient and cost effective catalysts for hydrogen generation from aqueous solution of ammonia borane (NH 3 BH 3 , AB) at room temperature . It is found that the as-synthesized NiM NPs (M = Cr, Mo, W) exhibit much higher catalytic performance for the hydrolysis of AB as compared to that of pure Ni NPs. In addition, among all the Ni 1-x M x (M = Cr, Mo, W) NPs, the Ni 0.9 Cr 0.1 , Ni 0.9 Mo 0.1 , and Ni 0.8 W 0.2 NPs show the highest catalytic activities with the turnover frequency (TOF) values of 10.7, 27.3 and 25.0 mol H 2 (mol metal min) −1 , respectively. Remarkably, these optimized NiM catalysts can also perform efficiently in the hydrolysis of hydrazine borane (N 2 H 4 BH 3 , HB). The present low-cost and high-performance of the NiM catalysts system may encourage the practical application of AB and HB as the promising chemical hydrogen storage materials .
研究领域:
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
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
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2022
·
IF 7.139
Ye Zhang,Xia Kang,Dong-Xue Liu,Ze-Yu Chen
In recent years, hydrazine borane (HB) as an excellent hydrogen material has been extensively studied by researchers because of its substantial hydrogen content (15.4 wt%), favourable chemical stability, eco-friendliness and being easy to synthesize. With Higher activity, catalysts of HB dehydrogenation will undoubtedly be more desirable for practical applications. In this work, CoIr nanoparticles (NPs) are successfully immobilized on TiO 2 substrate, achieving outstanding catalytic performance and 100% conversion for HB dehydrogenation. Particularly, Co 0.6 Ir 0.4 /TiO 2 can complete the reaction for HB dehydrogenation at 323 K within 32 s (0.53 min), and shows a fairly high turnover frequency (TOF) value (5625 h −1 ), which is higher than the values achieved by most Ni-based catalysts reported so far in the same condition. This superior catalytic performance can be attributed to uniform dispersion of metal NPs with small size and strong interaction among the CoIr NPs and the substrate. It is unquestionable that our work will help to promote the use of HB as a promising hydrogen storage material for fuel cells.
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
Scientific Reports
·
2015
·Vol. 5
·期 1
·1-11
·
IF 5.578
Yao Qilu,Lu Zhang-Hui,Yang Kangkang,Chen Xiangshu,Zhu Meihua
Ultrafine ruthenium nanoparticles (NPs) within the mesopores of the SBA-15 have been successfully prepared by using a “double solvents” method, in which n -hexane is used as a hydrophobic solvent and RuCl 3 aqueous solution is used as a hydrophilic solvent. After the impregnation and reduction processes, the samples were characterized by XRD, TEM, EDX, XPS, N 2 adsorption-desorption and ICP techniques. The TEM images show that small sized Ru NPs with an average size of 3.0 ± 0.8 nm are uniformly dispersed in the mesopores of SBA-15. The as-synthesized Ru@SBA-15 nanocomposites (NCs) display exceptional catalytic activity for hydrogen generation by the hydrolysis of ammonia borane (NH 3 BH 3 , AB) and hydrazine borane (N 2 H 4 BH 3 , HB) at room temperature with the turnover frequency (TOF) value of 316 and 706 mol H 2 (mol Ru min) −1 , respectively, relatively high values reported so far for the same reaction. The activation energies ( E a ) for the hydrolysis of AB and HB catalyzed by Ru@SBA-15 NCs are measured to be 34.8 ± 2 and 41.3 ± 2 kJ mol −1 , respectively. Moreover, Ru@SBA-15 NCs also show satisfied durable stability for the hydrolytic dehydrogenation of AB and HB, respectively.
研究领域:
纳米催化
·
能源材料
·
无机化学
·
氢气储存与释放
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多相催化
✓ 已验证
DOI
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
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
Journal of Materials Chemistry A
·
2020
·Vol. 8
·期 27
·13694-13701
·
IF 11.301
Wei Wang,Xiaoling Hong,Qilu Yao,Zhang-Hui Lu
In this work, mesoporous N-doped carbon (MNC) materials have been successfully prepared by a nanocasting route using SBA-15 as the template and ethylenediamine (EDA) and carbon tetrachloride (CTC) as carbon nitride precursors. The specific surface area and pore size of the MNC, as well as the C/N content are strongly dependent on the pyrolysis temperature. The as-obtained MNC-supported NiPt nanoparticles (NPs) were used as efficient catalysts toward complete dehydrogenation of hydrazine borane (HB) in alkaline solution at room temperature. Among all the catalysts investigated, the Ni60Pt40/MNC-800 nanocomposites (NCs) show the highest catalytic activity and 100% hydrogen selectivity. The total turnover frequency (TOF) of Ni60Pt40/MNC-800 NCs reached 1111 h−1 at room temperature, the highest activity among all catalysts reported to date. The superior catalytic properties were possibly a result of the electronic interaction between Ni and Pt, the synergistic effects of the NiPt NPs and MNC support, the ordered pore structure for free mass transfer and the small-sized metal NPs.
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
高影响因子
CATALYSIS TODAY
·
2021
·
IF 6.766
Qilu Yao,Jianjun Long,Kangkang Yang,Xiugang Li,Bin Huang,Xiangshu Chen,Zhang-Hui Lu
Designing highly active and selective metal nanocatalysts for use in liquid chemical hydrides is highly attractive but remains a critical challenge. Herein, bimetallic NiPt nanoparticles (NPs) immobilized on lanthanum oxycarbonate (NiPt/La 2 O 2 CO 3 ) have been facilely synthesized via an alkali-assisted reduction method. The introduction of NaOH is the key factor to the formation of the well-dispersed and ultrafine NiPt NPs (2.8 nm). The obtained Ni 0.6 Pt 0.4 /La 2 O 2 CO 3 exhibits an extraordinarily high catalytic activity and 100% H 2 selectivity for hydrous hydrazine dehydrogenation , providing a turnover frequency value (TOF) high up to 490 h −1 at 298 K. Additionally, the NiPt/La 2 O 2 CO 3 prepared with NaOH demonstrates higher catalytic performance and lower activation energy than that of NiPt/La 2 O 2 CO 3 _N prepared without NaOH. Moreover, the NiPt/La 2 O 2 CO 3 also shows an outstanding catalytic efficiency (TOF = 1200 h −1 ) for dehydrogenation of hydrazine borane at 298 K. The efficient catalytic performance may be attributed to the small size effect, the strong metal-support interaction, and the NaOH promotion effect. This alkali-assisted reduction method provides a new perspective for preparing of highly efficient catalysts in clean energy application.
研究领域:
材料科学
·
催化化学
·
清洁能源
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）