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Inorganic Chemistry Frontiers · 2019 ·Vol. 6 ·期 10 ·2727-2735 · IF 5.934

NiFePd/UiO-66 nanocomposites as highly efficient catalysts to accelerate hydrogen evolution from hydrous hydrazine

Xue Song,Pan Yang,Jingchuan Wang,Xiaochong Zhao,Yuanlin Zhou,Yintao Li,Lijun Yang

The exploration of highly efficient catalysts for the hydrolysis of hydrous hydrazine is of great significance for the achievement of future hydrogen economy. In this regard, herein, a catalyst with NiFePd loaded on the metal–organic framework (MOF) UiO-66 was successfully prepared by a simple and safe chemical impregnation method. Due to its high specific surface area, the as-prepared NiFePd/UiO-66 catalyst exhibited efficient catalytic performance for the generation of hydrogen from hydrous hydrazine in an alkaline solution. The results showed that the Ni0.25Fe0.25Pd0.5/UiO-66 catalyst exhibited optimal properties for the decomposition of hydrous hydrazine in an alkaline aqueous solution with a nearly 100% hydrogen selectivity, good activity, and the high total turnover frequency (TOF) value of up to 662.4 h−1 at 80 °C. Moreover, the Ni0.25Fe0.25Pd0.5/UiO-66 catalyst exhibited good durability, which slightly decreased after five cycles of catalytic reaction at 60 °C.

研究领域: 材料科学 · 催化化学 · 能源化学
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NANOTECHNOLOGY · 2016 ·Vol. 27 ·期 14 ·145701 · IF 3.573

Synthesis of TiO2-loaded Co0.85Se thin films with heterostructure and their enhanced catalytic activity for p-nitrophenol reduction and hydrazine hydrate decomposition

Yong Zuo,Ji-Ming Song,He-Lin Niu,Chang-Jie Mao,Sheng-Yi Zhang,Yu-Hua Shen

P-nitrophenol (4-NP) and hydrazine hydrate are considered to be highly toxic pollutants in wastewater, and it is of great importance to remove them. Herein, TiO2-loaded Co0.85Se thin films with heterostructure were successfully synthesized by a hydrothermal route. The as-synthesized samples were characterized by x-ray diffraction, x-ray photoelectron spectroscopy, transmission electron microscopy and selective-area electron diffraction. The results demonstrate that TiO2 nanoparticles with a size of about 10 nm are easily loaded on the surface of graphene-like Co0.85Se nanofilms, and the NH3 · H2O plays an important role in the generation and crystallization of TiO2 nanoparticles. Brunauer–Emmett–Teller measurement shows that the obtained nanocomposites have a larger specific surface area (199.3 m2 g−1) than that of Co0.85Se nanofilms (55.17 m2 g−1) and TiO2 nanoparticles (19.49 m2 g−1). The catalytic tests indicate Co0.85Se–TiO2 nanofilms have the highest activity for 4-NP reduction and hydrazine hydrate decomposition within 10 min and 8 min, respectively, compared with the corresponding precursor Co0.85Se nanofilms and TiO2 nanoparticles. The enhanced catalytic performance can be attributed to the larger specific surface area and higher rate of interfacial charge transfer in the heterojunction than that of the single components. In addition, recycling tests show that the as-synthesized sample presents stable conversion efficiency for 4-NP reduction.

研究领域: 材料科学 · 环境科学 · 化学
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CHEMISTRY-A EUROPEAN JOURNAL · 2018 ·Vol. 24 ·期 19 ·4902-4908 · IF 5.16

Tuning the Surface Composition of Ni/meso-CeO2 with Iridium as an Efficient Catalyst for Hydrogen Generation from Hydrous Hydrazine

Yu-Ping Qiu,Hui Yin,Hao Dai,Li-Yong Gan,Hong-Bin Dai,Ping Wang

Graphical Are two metals better than one? Surface modification of a Ni nanocatalyst by Ir results in remarkably improved catalytic properties towards H 2 generation from N 2 H 4 ⋅ H 2 O. Coupled experimental and theoretical studies reveal that the formation of Ni−Ir alloy on the catalyst surface plays a crucial role in determining the catalytic performance (see figure). Selective decomposition of hydrous hydrazine (N 2 H 4 ⋅ H 2 O) over metal catalysts provides a promising means for onboard or portable hydrogen source applications. Studies on N 2 H 4 ⋅ H 2 O decomposition catalysts mainly focus on the effects of bulk composition and structure on their performances, instead of the surface-composition-dependent properties. Herein, the synthesis of an Ir-modified Ni/ meso -CeO 2 catalyst is reported by using a combination of colloidal solution combustion synthesis and galvanic replacement methods. A combination of structural characterization, control experiments, and DFT calculations reveals that the Ni−Ir alloy resulting from calcination treatment exerts a profound effect on the catalytic properties. The resulting Ni@Ni−Ir/ meso -CeO 2 catalyst shows excellent catalytic performance towards hydrogen generation from N 2 H 4 ⋅ H 2 O, which compares favorably with the Ni−Ir bimetallic catalysts reported to date.

研究领域: 材料科学 · 催化化学 · 理论计算化学
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NEW JOURNAL OF CHEMISTRY · 2023 ·Vol. 47 ·期 16 ·7583-7587 · IF 3.3

The reaction kinetics and mechanism of catalytic decomposition of hydrazine nitrate on Ru/C catalyst in nitric acid solutions

Baole Li,Tiansheng He,Chen Zuo,Zhi Cao,Taihong Yan,Weifang Zheng

Catalytic decomposition of hydrazine nitrate is a very important research topic in the environmental protection field. Herein, we used an Ru/C catalyst for the decomposition of hydrazine nitrate in HNO3, and the reaction kinetics and mechanism were studied in detail. The kinetics study of the decomposition of hydrazine nitrate (0.01 M) was conducted in the temperature range 313–343 K in 0.1 M HNO3 in the presence of Ru/C. The apparent activation energy for this reaction was 46.6 kJ mol−1 according to a fitting of the experimental data, while the reaction order was 1.5. It was also found that the reaction pathway of the catalytic decomposition of hydrazine nitrate on the Ru/C catalyst involved two processes: heterogeneous catalytic disproportionation of hydrazine nitrate at the catalyst surface and oxidation of hydrazine nitrate with catalytically generated HNO2.

CAS / MDL: 7697-37-2
研究领域: 环境科学 · 催化化学
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2021 · IF 3.764

CuNi/La2O2CO3/rGO Nanocomposites: An Efficient Noble-Metal-Free Catalyst for Hydrogen Evolution from N2H4·H2O

Xiaoling Hong,Qilu Yao,Jianjun Long,Xiugang Li,Xiangshu Chen,Zhang-Hui Lu

Hydrous hydrazine (N2H4·H2O) has great potential as a convenient and safe hydrogen source for fuel cells. Tremendous efforts have been made to develop economic and efficient metal catalysts for hydrogen evolution from N2H4·H2O, but it remains a huge challenge. Herein, for the first time, noble-metal-free CuNi nanoparticles (NPs) immobilized on lanthanum oxycarbonate/reduced graphene oxide nanocomposites (CuNi/La2O2CO3/rGO) were successfully fabricated through an impregnation-reduction approach. Well-dispersed and ultrafine CuNi alloy NPs (∼3.2 nm) can be easily anchored onto La2O2CO3/rGO, and the aggregation of metal NPs can be effectively avoided. Benefiting from the small metal NP size, the synergistic effect between Cu and Ni, and the strong metal–support interactions, the Cu0.5Ni0.5/La2O2CO3/rGO nanocomposites (NCs) exhibited remarkably improved catalytic activity and 100% H2 selectively toward N2H4 decomposition, outperforming Cu/La2O2CO3/rGO, Ni/La2O2CO3/rGO, CuNi/rGO, and CuNi/La2O2CO3. The total turnover frequency of Cu0.5Ni0.5/La2O2CO3/rGO catalyst reached up to 114.3 h–1 at 343 K, indicating that the Cu0.5Ni0.5/La2O2CO3/rGO is one of the most active noble-metal-free catalysts ever reported for the same reaction. The low-cost and outstanding catalytic activity of CuNi/La2O2CO3/rGO NCs improved the feasibility of using N2H4·H2O as a chemical hydrogen carrier and is expected to be applied in economic hydrogen-based fuel cells.

CAS / MDL: 7803-57-8
研究领域: 材料科学 · 催化化学
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JOURNAL OF POWER SOURCES · 2015 · IF 6.217

Highly efficient Ni@Ni–Pt/La2O3 catalyst for hydrogen generation from hydrous hydrazine decomposition: Effect of Ni–Pt surface alloying

Yu-Jie Zhong,Hong-Bin Dai,Yuan-Yuan Jiang,De-Min Chen,Min Zhu,Li-Xian Sun,Ping Wang

Hydrous hydrazine has received increasing attention as a promising hydrogen carrier owing to its many favorable attributes, such as high hydrogen content, low material cost, stable liquid state at ambient conditions, and free of solid decomposition byproduct. Herein, we report the synthesis of a supported core–shell structured Ni@Ni–Pt/La 2 O 3 catalyst by a combination of co-precipitation and galvanic replacement methods. The catalyst exhibits high catalytic activity and 100% selectivity towards hydrogen generation from hydrous hydrazine at mild conditions, which outperforms most reported hydrous hydrazine decomposition catalysts. The favorable catalytic performance of the Ni@Ni–Pt/La 2 O 3 catalyst is correlated with the Pt-induced electronic and geometric modifications on the catalyst surface .

研究领域: 催化 · 材料科学 · 能源
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MATERIALS RESEARCH BULLETIN · 2024 · IF 5.3

Synthesis and catalytic properties of highly porous Ag-Rh nanocages

Huiyi Fang,Jin Xu,Tangyin Cui,Li Bai,Jiawei Meng,Chuncheng Wei,Xin Geng,Xiaowei Li,Haibin Sun,Guangwu Wen,Peng Wang

Ag-Rh nanocages are synthesised by a facile method at 190 °C using Ag nanocubes and Na 3 RhCl 6 as sacrificial templates and precursor, respectively. Upon introduction of Na 3 RhCl 6 into Ag nanocube suspension in ethylene glycol (EG) with poly(vinylpyrrolidone), Rh(III) ions are reduced by EG and Ag atoms via galvanic reaction; simultaneously, the released Ag(I) ions are reduced by EG. The reduction and co-deposition of both Ag and Rh atoms result in the formation of highly porous Ag-Rh nanocages when high volume of Na 3 RhCl 6 is introduced. The Ag-Rh nanocages with Ag:Rh atomic ratio of 54.2:45.8 exhibit good catalytic activity toward the degradation of rhodamine 6G, reduction of 4-nitrophenol, and decomposition of hydrazine.

CAS / MDL: 107-21-1
研究领域: 材料科学 · 催化 · 纳米技术
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2020 · IF 4.939

Mo-doped Ni-based catalyst for remarkably enhancing catalytic hydrogen evolution of hydrogen-storage materials

Yutong Wang,Lun Pan,Yixin Chen,Guoqiang Shen,Li Wang,Xiangwen Zhang,Ji-Jun Zou

Ni-based alloys are considered as the efficient catalyst for hydrogen-storage materials decomposition. Herein, we applied an in-situ melt-quenching method to dope Mo in Ni-based alloy for catalytic hydrogen evolution from hydrogen-storage materials. Importantly, Mo doped Ni-based catalyst exhibits more than 6 times higher TOF value than that of pure Ni both in AB hydrolysis and hydrazine decomposition, because Mo acts as an electron donor to improve the reducibility of Ni. Hydrogen evolution kinetics were studied over a range of temperatures (303–353 K) and initial feed concentrations (catalyst/hydrogen-storage materials (wt/wt) ratios = 0.2–10). Under optimal reaction conditions, the H 2 evolution rate reaches 1.92 mol H 2 /(mol cat  min) and 0.05 mol H 2 /(mol cat  min) in the hydrolysis of ammonia borane and decomposition of hydrazine, which are 6.42 and 6.44 times higher than undoped Ni catalyst, respectively. And the apparent activation energy of ammonia borane hydrolysis and hydrazine decomposition were evaluated to be 26.66 ± 3.31 kJ/mol and 40.01 ± 3.38 kJ/mol, respectively.

CAS / MDL: 13774-81-7
研究领域: 材料科学 · 催化化学
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