过渡金属氟化物对Mg-Al合金储氢性能的改性研究
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摘要
采用热处理工艺并结合机械合金化制备Mg-Al合金,研究过渡金属氟化物(TiF_3、VF_4以及ZrF_4)的添加对Mg-Al合金储氢性能的影响。研究发现,所有合金均主要由Mg_(17)Al_(12)相组成,Mg_(17)Al_(12)的氢化产物为MgH_2和Al,在过渡金属氟化物的催化作用下,Mg-Al合金的综合储氢性能得到明显提高。Mg-Al合金的初始吸/放氢温度约为180和300℃,添加TiF_3、VF_4以及ZrF_4后,合金的初始吸氢温度分别下降了80,30和30℃,初始放氢温度则分别下降了80,80和25℃,其中TiF_3显示出了良好的催化性能,尤其是在Mg-Al合金添加TiF_3后,Mg-Al合金氢化物的吸氢反应焓和脱氢反应焓从59.9和84.2 kJ/mol分别下降到了到了45.8和55.4 kJ/mol。
Mg-Al alloy was prepared by heat treatment combined with mechanical alloying, and the effect of transition metal fluoride on hydrogen storage performance of Mg-Al alloy was studied. It was found that the Mg-Al alloy was mainly composed of Mg_(17)Al_(12), and the hydrogenation products of Mg_(17)Al_(12) were MgH_2 and Al. Under the catalytic action of transition metal fluoride, the comprehensive hydrogen storage performance of Mg-Al alloy was obviously improved. The initial hydrogen absorption/desorption temperature of Mg-Al alloy was about 180 and 300 ℃. When TiF_3, VF_4 and ZrF_4 was added, those temperatures of the alloy decreased by 80, 30, 30 and 80, 80, 25 ℃, respectively. The results indicate that TiF_3 had the best catalytic effect on hydrogen storage of Mg-Al alloy. In particular, after the addition of TiF_3 to the Mg-Al alloy, the formation enthalpy of hydrogenation/dehydrogenation of the Mg-Al alloy hydride decreased from 59.9 and 84.2 kJ/mol to 45.8 and kJ/mol, respectively.
Mg-Al alloy was prepared by heat treatment combined with mechanical alloying, and the effect of transition metal fluoride on hydrogen storage performance of Mg-Al alloy was studied. It was found that the Mg-Al alloy was mainly composed of Mg_(17)Al_(12), and the hydrogenation products of Mg_(17)Al_(12) were MgH_2 and Al. Under the catalytic action of transition metal fluoride, the comprehensive hydrogen storage performance of Mg-Al alloy was obviously improved. The initial hydrogen absorption/desorption temperature of Mg-Al alloy was about 180 and 300 ℃. When TiF_3, VF_4 and ZrF_4 was added, those temperatures of the alloy decreased by 80, 30, 30 and 80, 80, 25 ℃, respectively. The results indicate that TiF_3 had the best catalytic effect on hydrogen storage of Mg-Al alloy. In particular, after the addition of TiF_3 to the Mg-Al alloy, the formation enthalpy of hydrogenation/dehydrogenation of the Mg-Al alloy hydride decreased from 59.9 and 84.2 kJ/mol to 45.8 and kJ/mol, respectively.
引文
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[3] Ismail M, Yap F A H, Yahya M S. Improved hydrogen storage properties of Mg-Li-Al-H composite system by milling with Fe2O3 powder [J]. Advanced Powder Technology, 2017, 28(9):2151-2158.
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[6] Lan Zhiqiang, Lyu Shaoxia, Zeng Ke, et al.The effect of Li and Li-based compound additions on the hydrogen storage properties of 17Mg/12Al composite [J].Journal of Functional Materials,2016,47(11):11076-11080(in Chinese).蓝志强, 吕韶霞, 曾科, 等. Li以及Li化合物的添加对17Mg/12Al复合材料储氢性能影响的研究[J]. 功能材料, 2016, 47(11): 11076-11080.
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[8] Tan X, Wang L, Holt C M B, et al. Body centered cubic magnesium niobium hydride with facile room temperature absorption and four weight percent reversible capacity [J]. Physical Chemistry Chemical Physics, 2012, 14(31):10904-10909.
[9] Chen C, Wang J, Wang H, et al. Improved kinetics of nanoparticle-decorated Mg-Ti-Zr nanocomposite for hydrogen storage at moderate temperatures [J]. Materials Chemistry and Physics, 2018, 206:21-28.
[10] Fadonougbo J O, Jung J Y, Suh J Y, et al. Low temperature formation of Mg2FeH6 by hydrogenation of ball-milled nano-crystalline powder mixture of Mg and Fe [J]. Materials & Design 2017, 135: 239-245.
[11] Zhang L T, Chen L X, Fan X L, et al. Enhanced hydrogen storage properties of MgH2 with numerous hydrogen diffusion channels provided by Na2Ti3O7 nanotubes [J]. Journal of Materials Chemistry A, 2017, 5(13):6178-6185.
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[13] Malka I E, Czujko T, Bystrzycki J. Catalytic effect of halide additives ball milled with magnesium hydride [J]. International Journal of Hydrogen Energy, 2010, 35(4):1706-1712.
[14] Khatabi M E l, Bhihi M, Naji S, et al. Study of doping effects with 3d and 4d-transition metals on the hydrogen storage properties of MgH2 [J]. International Journal of Hydrogen Energy, 2016, 41(8):4712-4718.
[15] Chen B H, Chuang Y S, Chen C K. Improving the hydrogenation properties of MgH2 at room temperature by doping with nano-size ZrO2 catalyst [J]. Journal of Alloys and Compounds, 2016, 655:21-27.
[16] Long S, Zou J, Chen X, et al. A comparison study of Mg-Y2O3 and Mg-Y hydrogen storage composite powders prepared through arc plasma method [J]. Journal of Alloys and Compounds, 2014, 615:S684-S688.
[17] Peng W, Lan Z, Wei W, et al. Investigation on preparation and hydrogen storage performance of Mg17Al12 alloy [J]. International Journal of Hydrogen Energy, 2016, 41(3):1759-1765.
[18] Zhong H C, Wang H, Ouyang L Z. Improving the hydrogen storage properties of MgH2 by reversibly forming Mg-Al solid solution alloys [J]. International Journal of Hydrogen Energy, 2014, 39(7):3320-3326.
[19] Lan Z, Peng W, Wei W, et al. Preparation and hydrogen storage properties of Mg-Al-Li solid solution [J]. International Journal of Hydrogen Energy, 2016, 41(14):6134-6138.
[20] Shahi R R, Bhatnagar A, Pandey S K, et al. Effects of Ti-based catalysts and synergistic effect of SWCNTs-TiF3 on hydrogen uptake and release from MgH2 [J]. International Journal of Hydrogen Energy, 2014, 39(26):14255-14261.
[21] Ma L P, Kang X D, Dai H B, et al. Superior catalytic effect of TiF3 over TiCl3 in improving the hydrogen sorption kinetics of MgH2: catalytic role of fluorine anion [J]. Acta Materialia, 2009, 57(7):2250-2258.
[22] Wu H, Du J, Cai F, et al. Catalytic effects of V and V2O5 on hydrogen storage property of Mg17Al12 alloy [J]. International Journal of Hydrogen Energy, 2018, 43(31):14578-14583.
[23] Wang Y Q, Lyu S X, Zhou Z Y, et al. Effect of transition metal on the hydrogen storage properties of Mg-Al alloy [J]. Journal of Materials Science, 2017, 52(5):2392-2399.
[2] Xu Yixin, Xiao Xuezhang. Investigation of catalytic modification of light magnesium based hydrogen storage material [J]. Journal of Functional Materials, 2015,46(7):7135-7137(in Chinese).许以欣, 肖学章. 轻质镁基储氢材料的高效催化改性研究[J]. 功能材料, 2015, 46(7): 7135-7137.
[3] Ismail M, Yap F A H, Yahya M S. Improved hydrogen storage properties of Mg-Li-Al-H composite system by milling with Fe2O3 powder [J]. Advanced Powder Technology, 2017, 28(9):2151-2158.
[4] Lan Z, Sun Z, Ding Y, et al. Catalytic action of Y2O3@graphene nanocomposites on the hydrogen-storage properties of Mg-Al alloys [J]. Journal of Materials Chemistry A, 2017, 5(29):15200-15207.
[5] Wang Y, Lu S, Zhou Z, et al. Effect of transition metal on the hydrogen storage properties of Mg-Al alloy [J]. Journal of Materials Science, 2017, 52(5):2392-2399.
[6] Lan Zhiqiang, Lyu Shaoxia, Zeng Ke, et al.The effect of Li and Li-based compound additions on the hydrogen storage properties of 17Mg/12Al composite [J].Journal of Functional Materials,2016,47(11):11076-11080(in Chinese).蓝志强, 吕韶霞, 曾科, 等. Li以及Li化合物的添加对17Mg/12Al复合材料储氢性能影响的研究[J]. 功能材料, 2016, 47(11): 11076-11080.
[7] Luo X, Grant D M, Walker G S. Catalytic effect of nano-sized ScH2 on the hydrogen storage of mechanically milled MgH2 [J]. Journal of Alloys and Compounds, 2015, 622:842-850.
[8] Tan X, Wang L, Holt C M B, et al. Body centered cubic magnesium niobium hydride with facile room temperature absorption and four weight percent reversible capacity [J]. Physical Chemistry Chemical Physics, 2012, 14(31):10904-10909.
[9] Chen C, Wang J, Wang H, et al. Improved kinetics of nanoparticle-decorated Mg-Ti-Zr nanocomposite for hydrogen storage at moderate temperatures [J]. Materials Chemistry and Physics, 2018, 206:21-28.
[10] Fadonougbo J O, Jung J Y, Suh J Y, et al. Low temperature formation of Mg2FeH6 by hydrogenation of ball-milled nano-crystalline powder mixture of Mg and Fe [J]. Materials & Design 2017, 135: 239-245.
[11] Zhang L T, Chen L X, Fan X L, et al. Enhanced hydrogen storage properties of MgH2 with numerous hydrogen diffusion channels provided by Na2Ti3O7 nanotubes [J]. Journal of Materials Chemistry A, 2017, 5(13):6178-6185.
[12] Gasan H, Celik O N, Aydinbeyli N, et al. Effect of V, Nb, Ti and graphite additions on the hydrogen desorption temperature of magnesium hydride [J]. International Journal of Hydrogen Energy, 2012, 37(2):1912-1918.
[13] Malka I E, Czujko T, Bystrzycki J. Catalytic effect of halide additives ball milled with magnesium hydride [J]. International Journal of Hydrogen Energy, 2010, 35(4):1706-1712.
[14] Khatabi M E l, Bhihi M, Naji S, et al. Study of doping effects with 3d and 4d-transition metals on the hydrogen storage properties of MgH2 [J]. International Journal of Hydrogen Energy, 2016, 41(8):4712-4718.
[15] Chen B H, Chuang Y S, Chen C K. Improving the hydrogenation properties of MgH2 at room temperature by doping with nano-size ZrO2 catalyst [J]. Journal of Alloys and Compounds, 2016, 655:21-27.
[16] Long S, Zou J, Chen X, et al. A comparison study of Mg-Y2O3 and Mg-Y hydrogen storage composite powders prepared through arc plasma method [J]. Journal of Alloys and Compounds, 2014, 615:S684-S688.
[17] Peng W, Lan Z, Wei W, et al. Investigation on preparation and hydrogen storage performance of Mg17Al12 alloy [J]. International Journal of Hydrogen Energy, 2016, 41(3):1759-1765.
[18] Zhong H C, Wang H, Ouyang L Z. Improving the hydrogen storage properties of MgH2 by reversibly forming Mg-Al solid solution alloys [J]. International Journal of Hydrogen Energy, 2014, 39(7):3320-3326.
[19] Lan Z, Peng W, Wei W, et al. Preparation and hydrogen storage properties of Mg-Al-Li solid solution [J]. International Journal of Hydrogen Energy, 2016, 41(14):6134-6138.
[20] Shahi R R, Bhatnagar A, Pandey S K, et al. Effects of Ti-based catalysts and synergistic effect of SWCNTs-TiF3 on hydrogen uptake and release from MgH2 [J]. International Journal of Hydrogen Energy, 2014, 39(26):14255-14261.
[21] Ma L P, Kang X D, Dai H B, et al. Superior catalytic effect of TiF3 over TiCl3 in improving the hydrogen sorption kinetics of MgH2: catalytic role of fluorine anion [J]. Acta Materialia, 2009, 57(7):2250-2258.
[22] Wu H, Du J, Cai F, et al. Catalytic effects of V and V2O5 on hydrogen storage property of Mg17Al12 alloy [J]. International Journal of Hydrogen Energy, 2018, 43(31):14578-14583.
[23] Wang Y Q, Lyu S X, Zhou Z Y, et al. Effect of transition metal on the hydrogen storage properties of Mg-Al alloy [J]. Journal of Materials Science, 2017, 52(5):2392-2399.