通过添加酒石酸配体制备了使双金属催化剂中不同组分配合比的可调节非晶态合金催化剂,并对合成的镍-铁-硼-酒石酸(Ni-Fe-B-ta)双金属纳米颗粒进行了表征,其比表面积为100.54m2/g。同时研究了催化剂在硼氢化钠(NaBH4)水解制氢中的催化活性。研究结果表明,添加酒石酸同时调控2种金属的催化剂大大提高了NaBH4水解产氢的能力,其最高产氢速率达到7300mL/(min·g),活化能为46.0kJ/mol,经过3次重复催化后,该催化剂依然可以保持较高的催化活性。
An amorphous alloy catalyst with adjustable ratio of different components in the bimetallic catalyst was prepared by adding tartaric acid ligand.The synthesized Ni-Fe-B-ta bimetallic nanoparticles were characterized.And the Ni-Fe-B-ta had an estimated Langmuir surface erea of 100.54m2/g.The catalytic activity was also studied by catalyzing hydrogen hydrolysis of sodium borohydride.The experimental results shown that the addition of tartaric acid to the catalysts of both metals greatly improved the ability of NaBH4 to produce hydrogen,and the maximum hydrogen production rate at room temperature reached 7300mL/(min·g) with an activation energy of 46.0kJ/mol.The cyclic test results shown that after 3 repeated catalytic tests,the catalyst can still maintain a high catalytic activity.
[1] 孙海杰,黄振旭,王雅苹,等.非晶态合金Ru-B/ZrO2催化剂催化硼氢化钠水解制氢性能的研究[J].化工新型材料,2018,46(1):102-105.
[2] 徐东彦,张华民,叶威.硼氢化钠水解制氢[J].化学进展,2007,19(10):1598-1605.
[3] 杨兰,罗威,程功臻.氨硼烷水解制氢的研究进展[J].大学化学,2014,29(6):1-10.
[4] Tang M Y,Xia F L,Gao C J,et al.Preparation of magnetically recyclable CuFe2O4/RGO for catalytic hydrolysis of sodium borohydride[J].International Journal of Hydrogen Energy,2016,41(30):13058-13068.
[5] Jadhav A R,Bandal H A,Kim H.NiCo2O4 hollow sphere as an efficient catalyst for hydrogen generation by NaBH4 hydrolysis[J].Materials Letters,2017,198:50-53.
[6] Brack P,Dann S E,Wijayantha K G U.Heterogeneous and homogenous catalysts for hydrogen generation by hydrolysis of aqueous sodium borohydride (NaBH4) solutions[J].Energy Science & Engineering,2015,3:174-188.
[7] Kim D R,Cho K W,Choi Y Il,et al.Fabrication of porous Co-Ni-P catalysts by electrodeposition and their catalytic characteristics for the generation of hydrogen from an alkaline NaBH4 solution[J].International Journal of Hydrogen Energy,2009,34(6):2622-2630.
[8] Patel N,Fernandes R,Miotello A.Promoting effect of transition metal-doped Co-B alloy catalysts for hydrogen production by hydrolysis of alkaline NaBH4 solution[J].Journal of Catalysis,2010,271(2):315-324.
[9] Glezer A M,Gorshenkov M V,Zhukov D G,et al.Pinning of nanocrystals growth at Fe-Ni-B amorphous alloy crystallization:atom probe investigations[J].Materials Letters,2015,160:339-342.
[10] Tsai C W,Chen H M,Liu R S,et al.Magnetically recyclable Fe@Co core-shell catalysts for dehydrogenation of sodium borohydride in fuel cells[J].International Journal of Hydrogen Energy,2012,37(4):3338-3343.
[11] Bandal H A,Jadhav A R,Kim H.Cobalt impregnated magnetite-multiwalled carbon nanotube nanocomposite as magnetically separable efficient catalyst for hydrogen generation by NaBH4 hydrolysis[J].Journal of Alloys and Compounds,2017,699:1057-1067.
[12] 黄珍霞,梁峰,张海军,等.含Co或Ni的双金属及三金属纳米颗粒的制备方法及其催化制氢性能[J].化学通报,2017,80(7):621-630.
[13] Zhang H,Okumura M,Toshima N.Stable dispersions of PVP-Protected Au/Pt/Ag trimetallic nanoparticles as highly active colloidal catalysts for aerobic glucose oxidation[J].Journal of Physical Chemistry C,2011,115(30):14883-14891.
[14] Zhang H,Haba M,Okumura M,et al.Novel formation of Ag/Au bimetallic nanoparticles by physical mixture of monometallic nanoparticles in dispersions and their application to catalysts for aerobic glucose oxidation[J].Langmuir,2013,29(33):10330-10339.
[15] Zhang H,Toshima N.Glucose oxidation using Au-containing bimetallic and trimetallic nanoparticles[J].Catalysis Science Technology,2013,3:268-278.
[16] Wu C,Bai Y,Liu D X,et al.Ni-Co-B catalyst-promoted hydrogen generation by hydrolyzing NaBH4 solution for in situ hydrogen supply of portable fuel cells[J].Catalysis Today,2011,170(1):33-39.
[17] Nie M,Zou Y C,Huang Y M,et al.Ni-Fe-B catalysts for NaBH4 hydrolysis[J].International Journal of Hydrogen Energy,2012,37(2):1568-1576.
[18] Guo J,Hou Y J,Yang C H,et al.Effects of nickel ethylenediamine complex on the preparation of Ni-B amorphous alloy catalyst with ultrasonic assistance[J].Materials Letters,2012,67(1):151-153.
[19] Wonterghem J,Morup S,Koch C J W,et al.Formation of ultra-fine amorphous alloy particles by reduction in aqueous solution[J].Nature,1986,322:622-623.
[20] He Y,Qiao M,Hu H,et al.Characterization and catalytic behavior of amorphous Ni-B/AC catalysts prepared in different impregnation sequences[J].Applied Catalysis A,2002,228(1/2):29-37.
[21] Li H,Li H X,Deng J F.Glucose hydrogenation over Ni-B/SiO2 amorphous alloy catalyst and the promoting effect of metal dopants[J].Catalysis Today,2002,74(1/2):53-63.
[22] Guo J,Hou Y J,Yang C H,et al.Preparation of Ni-B amorphous alloy catalyst from nickel hydrazine complex with ultrasonic assistance[J].Catalysis Communications,2011,16(1):86-89.
[23] Xiong Y,Siekkinen A R,Wang J,et al.Synthesis of silver nanoplates at high yields by slowing down the polyol reduction of silver nitrate with polyacrylamide[J].Materials Chemistry and Physics,2007,17:2600-2602.
[24] Fang J,Chen X Y,Liu B,et al.Liquid-phase chemoselective hydrogenation of 2-ethylanthraquinone over chromium-modified nanosized amorphous Ni-B catalysts[J].Journal of Catalysis,2005,229(1):97-104.
[25] Li H,Li H X,Deng J F.The crystallization process of ultrafine Ni-B amorphous alloy[J].Materials Letters,2001,50(1):41-46.
基金资助
河北省自然科学基金项目(B2018208188);河北省人社厅留学人员科技活动项目(CL201610);河北省重大科技成果转化专项项目(18041409Z)
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