The fullerene complex, η 2 C 60 [Ru(NO)(PPh 3)] 2, has been prepared by the reaction of C 60 with Ru(NO) 2(PPh 3) 2 under a nitrogen atmosphere and refluxing. The new complex was characterized by means of elemental a...The fullerene complex, η 2 C 60 [Ru(NO)(PPh 3)] 2, has been prepared by the reaction of C 60 with Ru(NO) 2(PPh 3) 2 under a nitrogen atmosphere and refluxing. The new complex was characterized by means of elemental analysis, IR, XPS, electronic spectra and 31 P NMR. The results show that the complex of η 2 form can be formed by C 60 bonding to Ru(NO) 2(PPh 3) 2 in the σ π way and there is hyperconjugation effect in the molecule. So electrons will flow easier and photoelectric effect for this new compound is expected. In addition, the structure of the complex has been supposed. The ruthenium is 4 coordinate in the complex, bonding to two carbon atoms, to one PPh 3 and to one NO.展开更多
氮化硅是一种良好的载体,具有较高的水热稳定性和机械稳定性,其表面的氨基基团能够较好地锚定金属,显著提高金属分散度。但是,商品氮化硅比表面积较低,对金属分散作用仍然有限。因此,以自制的高比表面积氮化硅(Si_(3)N_(4))为载体,通过...氮化硅是一种良好的载体,具有较高的水热稳定性和机械稳定性,其表面的氨基基团能够较好地锚定金属,显著提高金属分散度。但是,商品氮化硅比表面积较低,对金属分散作用仍然有限。因此,以自制的高比表面积氮化硅(Si_(3)N_(4))为载体,通过浸渍法制备了不同Ru负载量(质量分数分别为0.5%、1.0%和2.0%)的催化剂(分别为0.5%Ru/Si_(3)N_(4)、1.0%Ru/Si_(3)N_(4)和2.0%Ru/Si_(3)N_(4)),并以商品氮化硅(Si_(3)N_(4)-C)为载体制备了2.0%Ru/Si_(3)N_(4)-C催化剂作为对照组。表征了催化剂的理化性质,测试了其在300℃、0.1 MPa下的CO_(2)加氢反应活性。结果显示,与Si_(3)N_(4)-C相比,Si_(3)N_(4)的比表面积较高(502 m^(2)/g),Si_(3)N_(4)作为载体显著提高了金属分散度,降低了金属粒径,催化剂暴露出更多的活性位点。0.5%Ru/Si_(3)N_(4)的金属粒径较小,展现出强的H_(2)吸附能力,H难以解吸,抑制了中间物种CO加氢生成CH_(4)。随着Ru负载量增加,金属粒径增大,催化剂的CH_(4)选择性更好。Ru/Si_(3)N_(4)系列催化剂中,2.0%Ru/Si_(3)N_(4)的CH_(4)选择性较高(98.8%)。空速为10000 m L/(g·h)时,0.5%Ru/Si_(3)N_(4)的CO选择性为88.2%。与2.0%Ru/Si_(3)N_(4)相比,2.0%Ru/Si_(3)N_(4)-C的金属粒径更大,活性位点较少,活性更低。2.0%Ru/Si_(3)N_(4)和2.0%Ru/Si_(3)N_(4)-C的CO_(2)转化率分别为53.1%和9.2%。Si_(3)N_(4)有效提高了金属分散度,提高了催化剂的CO_(2)加氢反应活性;通过调控Ru负载量控制催化剂金属粒径,可实现对产物CO或CH_(4)选择性的调控。展开更多
The fullerene complex,C60 RuH2(CO)(PPh3),has been prepared and characterize d by elemental analyses,IR and electronic spectra.In addition,the redox property of t he complex has been studied by cyclic voltammetry.The r...The fullerene complex,C60 RuH2(CO)(PPh3),has been prepared and characterize d by elemental analyses,IR and electronic spectra.In addition,the redox property of t he complex has been studied by cyclic voltammetry.The results s how that the reduction potential of C60 RuH2(CO)(PPh3)is more negative than that of C60.Meanwhile,with the extent of the complex reduction get to increace the stability of the complex ion is on the decrease.展开更多
The title complex was obtained by reactions of [Mo(CO)_3(MeCN)_3] with [CuBr(pySH)(PPh_3)_2]or directly with pySH and PPh_3. The latter method can be used to synthesize the corresponding tungsten complex [W_2(CO)_4(μ...The title complex was obtained by reactions of [Mo(CO)_3(MeCN)_3] with [CuBr(pySH)(PPh_3)_2]or directly with pySH and PPh_3. The latter method can be used to synthesize the corresponding tungsten complex [W_2(CO)_4(μ-pyS)_2(PPh_3)_2].The molecular structure of the title compound was determined by X-ray diffraction method.展开更多
文摘The fullerene complex, η 2 C 60 [Ru(NO)(PPh 3)] 2, has been prepared by the reaction of C 60 with Ru(NO) 2(PPh 3) 2 under a nitrogen atmosphere and refluxing. The new complex was characterized by means of elemental analysis, IR, XPS, electronic spectra and 31 P NMR. The results show that the complex of η 2 form can be formed by C 60 bonding to Ru(NO) 2(PPh 3) 2 in the σ π way and there is hyperconjugation effect in the molecule. So electrons will flow easier and photoelectric effect for this new compound is expected. In addition, the structure of the complex has been supposed. The ruthenium is 4 coordinate in the complex, bonding to two carbon atoms, to one PPh 3 and to one NO.
文摘氮化硅是一种良好的载体,具有较高的水热稳定性和机械稳定性,其表面的氨基基团能够较好地锚定金属,显著提高金属分散度。但是,商品氮化硅比表面积较低,对金属分散作用仍然有限。因此,以自制的高比表面积氮化硅(Si_(3)N_(4))为载体,通过浸渍法制备了不同Ru负载量(质量分数分别为0.5%、1.0%和2.0%)的催化剂(分别为0.5%Ru/Si_(3)N_(4)、1.0%Ru/Si_(3)N_(4)和2.0%Ru/Si_(3)N_(4)),并以商品氮化硅(Si_(3)N_(4)-C)为载体制备了2.0%Ru/Si_(3)N_(4)-C催化剂作为对照组。表征了催化剂的理化性质,测试了其在300℃、0.1 MPa下的CO_(2)加氢反应活性。结果显示,与Si_(3)N_(4)-C相比,Si_(3)N_(4)的比表面积较高(502 m^(2)/g),Si_(3)N_(4)作为载体显著提高了金属分散度,降低了金属粒径,催化剂暴露出更多的活性位点。0.5%Ru/Si_(3)N_(4)的金属粒径较小,展现出强的H_(2)吸附能力,H难以解吸,抑制了中间物种CO加氢生成CH_(4)。随着Ru负载量增加,金属粒径增大,催化剂的CH_(4)选择性更好。Ru/Si_(3)N_(4)系列催化剂中,2.0%Ru/Si_(3)N_(4)的CH_(4)选择性较高(98.8%)。空速为10000 m L/(g·h)时,0.5%Ru/Si_(3)N_(4)的CO选择性为88.2%。与2.0%Ru/Si_(3)N_(4)相比,2.0%Ru/Si_(3)N_(4)-C的金属粒径更大,活性位点较少,活性更低。2.0%Ru/Si_(3)N_(4)和2.0%Ru/Si_(3)N_(4)-C的CO_(2)转化率分别为53.1%和9.2%。Si_(3)N_(4)有效提高了金属分散度,提高了催化剂的CO_(2)加氢反应活性;通过调控Ru负载量控制催化剂金属粒径,可实现对产物CO或CH_(4)选择性的调控。
文摘The fullerene complex,C60 RuH2(CO)(PPh3),has been prepared and characterize d by elemental analyses,IR and electronic spectra.In addition,the redox property of t he complex has been studied by cyclic voltammetry.The results s how that the reduction potential of C60 RuH2(CO)(PPh3)is more negative than that of C60.Meanwhile,with the extent of the complex reduction get to increace the stability of the complex ion is on the decrease.
文摘The title complex was obtained by reactions of [Mo(CO)_3(MeCN)_3] with [CuBr(pySH)(PPh_3)_2]or directly with pySH and PPh_3. The latter method can be used to synthesize the corresponding tungsten complex [W_2(CO)_4(μ-pyS)_2(PPh_3)_2].The molecular structure of the title compound was determined by X-ray diffraction method.
