采用硅烷偶联剂Z6020对六方氮化硼(h-BN)进行改性,通过原位聚合法制备聚酰亚胺/改性氮化硼(PI/f-BN)复合薄膜。利用红外光谱仪、自制调频耐电晕装置和宽频介电谱测试仪对复合薄膜进行测试,采用光学显微镜对薄膜耐电晕老化后的击穿孔形...采用硅烷偶联剂Z6020对六方氮化硼(h-BN)进行改性,通过原位聚合法制备聚酰亚胺/改性氮化硼(PI/f-BN)复合薄膜。利用红外光谱仪、自制调频耐电晕装置和宽频介电谱测试仪对复合薄膜进行测试,采用光学显微镜对薄膜耐电晕老化后的击穿孔形貌进行表征。结果表明:在棒板空气间隙为1 mm,脉冲电场强度为50 k V/mm,占空比为50%,频率为20 k Hz的测试条件下,随着f-BN含量的提高,薄膜的耐电晕寿命呈先增加后缩短的趋势。当f-BN含量为15%时,复合薄膜的介电常数最大,耐电晕寿命最长。展开更多
Synthesis of ultrafine noble metal with sizes down to nanoscale and even atomic scale is of great significance for heterogeneous catalysis. However, the metal loading is usually kept below 2 wt% due to the aggregation...Synthesis of ultrafine noble metal with sizes down to nanoscale and even atomic scale is of great significance for heterogeneous catalysis. However, the metal loading is usually kept below 2 wt% due to the aggregation tendency at higher metal contents. Herein, by mimicking the multicentered metal sulfur cluster of metalloenzyme, a bioinspired synthesis of isolated noble metal atoms on the metal-organic sulfide(MOS) framework was reported. The sulfur-rich framework featuring [Mo_(3)S_(2)Br_(6)]^(2-) cluster as the building block and dithiol as the linking node was constructed via chemical bonding and employed to support atomic metal species. Remarkably, highly dispersed platinum atoms with a loading amount as high as 18.5 wt% on the underlying sulfurrich framework could be obtained after reduction. By increasing the number of benzene rings in the dithiol, the pore size and even the wettability of the MOS frameworks could be modulated. The general applicability of the synthesis could also be extended to the synthesis of atomic Pd. Furthermore,the Pt-loaded MOS could serve as the catalyst for selective hydrogenation of phenylacetylene to styrene in both organic solvent and pure water. Density function theory calculation demonstrated that the atomic Pt sites in the sulfur-rich coordination environment could activate H_(2) molecules and chemoselectively catalyze the semi-hydrogenation of phenylacetylene to styrene through moderately low energy barriers.The metalation of such a versatile MOS framework will shed light on the synthesis of bioinspired catalytic materials with well-defined structures for more diverse applications.展开更多
文摘采用硅烷偶联剂Z6020对六方氮化硼(h-BN)进行改性,通过原位聚合法制备聚酰亚胺/改性氮化硼(PI/f-BN)复合薄膜。利用红外光谱仪、自制调频耐电晕装置和宽频介电谱测试仪对复合薄膜进行测试,采用光学显微镜对薄膜耐电晕老化后的击穿孔形貌进行表征。结果表明:在棒板空气间隙为1 mm,脉冲电场强度为50 k V/mm,占空比为50%,频率为20 k Hz的测试条件下,随着f-BN含量的提高,薄膜的耐电晕寿命呈先增加后缩短的趋势。当f-BN含量为15%时,复合薄膜的介电常数最大,耐电晕寿命最长。
基金financially supported by the National Natural Science Foundation of China (22175104, 21802080 and 21902082)the Natural Science Foundation of Shandong Province (ZR2019ZD47 and ZR2019JQ05)+1 种基金China Postdoctoral Science Foundation (2019M652341)the Education Department of Shandong Province (2019KJC006)。
文摘Synthesis of ultrafine noble metal with sizes down to nanoscale and even atomic scale is of great significance for heterogeneous catalysis. However, the metal loading is usually kept below 2 wt% due to the aggregation tendency at higher metal contents. Herein, by mimicking the multicentered metal sulfur cluster of metalloenzyme, a bioinspired synthesis of isolated noble metal atoms on the metal-organic sulfide(MOS) framework was reported. The sulfur-rich framework featuring [Mo_(3)S_(2)Br_(6)]^(2-) cluster as the building block and dithiol as the linking node was constructed via chemical bonding and employed to support atomic metal species. Remarkably, highly dispersed platinum atoms with a loading amount as high as 18.5 wt% on the underlying sulfurrich framework could be obtained after reduction. By increasing the number of benzene rings in the dithiol, the pore size and even the wettability of the MOS frameworks could be modulated. The general applicability of the synthesis could also be extended to the synthesis of atomic Pd. Furthermore,the Pt-loaded MOS could serve as the catalyst for selective hydrogenation of phenylacetylene to styrene in both organic solvent and pure water. Density function theory calculation demonstrated that the atomic Pt sites in the sulfur-rich coordination environment could activate H_(2) molecules and chemoselectively catalyze the semi-hydrogenation of phenylacetylene to styrene through moderately low energy barriers.The metalation of such a versatile MOS framework will shed light on the synthesis of bioinspired catalytic materials with well-defined structures for more diverse applications.
