Hexamethylenediamine(HMDA) is an important reagent for the synthesis of Nylon-6,6, and it is usually produced by the hydrogenation of adiponitrile using a toxic reagent of hydrocyanic acid. Herein, we developed an env...Hexamethylenediamine(HMDA) is an important reagent for the synthesis of Nylon-6,6, and it is usually produced by the hydrogenation of adiponitrile using a toxic reagent of hydrocyanic acid. Herein, we developed an environmental friendly route to produce HMDA via catalytic reductive amination of 1,6-hexanediol(HDO) in the presence of hydrogen. The activities of several heterogeneous metal catalysts such as supported Ni, Co, Ru, Pt, Pd catalysts were screened for the present reaction in supercritical ammonia without any additives. Among the catalysts examined, Ru/Al_2O_3 presented a high catalytic activity and highest selectivity for the desired product of HMDA. The high performance of Ru/Al_2O_3 was discussed based on the Ru dispersion and the surface properties like the acid-basicity. In addition, the reaction parameters such as reaction temperature,time, H_2 and NH_3 pressure were examined, and the reaction processes were discussed in detail.展开更多
Exploring and designing bi-functional catalysts with earth-abundant elements that can work well for both hydrogen evolution reaction（HER） and oxygen evolution reaction（OER） in alkaline medium are of significance f...Exploring and designing bi-functional catalysts with earth-abundant elements that can work well for both hydrogen evolution reaction（HER） and oxygen evolution reaction（OER） in alkaline medium are of significance for producing clean fuel to relieve energy and environment crisis.Here,a novel Ni/NiO monolithic electrode was developed by a facile and cost-effective acid promoted activation of Ni foam.After the treatment,this obtained monolithic electrode with a layer of NiO on its surface demonstrates rough and sheet-like morphology,which not only possesses larger accessible surface area but also provides more reactive active sites. Compared with powder catalysts,this monolithic electrode can achieve intimate contact between the electrocatalyst and the current collector,which will alleviate the problem of pulverization and enable the stable function of the electrode. It can be served as an efficient bi-functional electrocatalyst with an overpotential of 160 mV for HER and 290 mV for OER to produce current densities of 10 mA cm^（-2） in the alkaline medium. And it maintains benign stability after 5,000 cycles,which rivals many recent reported noble-metal free catalysts in 1.0mol L^（-1） KOH solution. Attributed to the easy,scalable methodology and high catalytic efficiency,this work not only offers a promising monolithic catalyst but also inspires us to exploit other inexpensive,highly efficient and self-standing noble metalfree electrocatalysts for scale-up electrochemical water-splitting technology.展开更多
Signal drift and performance instability of brain-computer interface devices induced by the interface failure between rigid metal electrodes and soft human skin hinder the precise data acquisition of electroencephalog...Signal drift and performance instability of brain-computer interface devices induced by the interface failure between rigid metal electrodes and soft human skin hinder the precise data acquisition of electroencephalogram(EEG).Thus,it is desirable to achieve a robust interface for brain-computer interface devices.Here,a kind of polydopamine methacrylamide-polyacrylamide(PDMA-PAAM)hydrogel is developed.To improve the adhesion,dopamine is introduced into the polyacrylamide hydrogel,through the amino and catechol groups of dopamine in an organic-inorganic interface to build a covalent and non-covalent interaction.A strong attachment and an effective modulus transition system can be formed between the metal electrodes and human skin,so that the peeling force between the PDMAPAAM hydrogel and the porcine skin can reach 22 N m^(-1).In addition,the stable conductivity and long-term operating life of the PDMA-PAAM hydrogel for more than 60 days at room temperature are achieved by adding sodium chloride(NaCl)and glycerol,respectively.The PDMA-PAAM hydrogel membrane fabricated in this work is integrated onto a flexible Au electrode applied in a brain-computer interface.In comparison,the collected EEG signal intensity and waveform are consistent with that of the commercial counterparts.And obviously,the flexible electrode with PDMA-PAAM hydrogel membrane is demonstrated to enable a more stable and userfriendly interface.展开更多
基金supported by the National Basic Research Program of China(2016YFA0602900)Youth Innovation Promotion Association CAS(2016206)Jilin Provincial Science and Technology Program of China(20150301012GX)
文摘Hexamethylenediamine(HMDA) is an important reagent for the synthesis of Nylon-6,6, and it is usually produced by the hydrogenation of adiponitrile using a toxic reagent of hydrocyanic acid. Herein, we developed an environmental friendly route to produce HMDA via catalytic reductive amination of 1,6-hexanediol(HDO) in the presence of hydrogen. The activities of several heterogeneous metal catalysts such as supported Ni, Co, Ru, Pt, Pd catalysts were screened for the present reaction in supercritical ammonia without any additives. Among the catalysts examined, Ru/Al_2O_3 presented a high catalytic activity and highest selectivity for the desired product of HMDA. The high performance of Ru/Al_2O_3 was discussed based on the Ru dispersion and the surface properties like the acid-basicity. In addition, the reaction parameters such as reaction temperature,time, H_2 and NH_3 pressure were examined, and the reaction processes were discussed in detail.
基金supported by the National Natural Science Foundation of China (21571073 and 21673090)the National Basic Research Program of China (2015CB932600)+2 种基金Hubei Provincial Natural Science Foundation of China (2016CFA031)the Program for HUST Interdisciplinary Innovation Team (2015ZDTD038)the Fundamental Research Funds for the Central Universities
文摘Exploring and designing bi-functional catalysts with earth-abundant elements that can work well for both hydrogen evolution reaction（HER） and oxygen evolution reaction（OER） in alkaline medium are of significance for producing clean fuel to relieve energy and environment crisis.Here,a novel Ni/NiO monolithic electrode was developed by a facile and cost-effective acid promoted activation of Ni foam.After the treatment,this obtained monolithic electrode with a layer of NiO on its surface demonstrates rough and sheet-like morphology,which not only possesses larger accessible surface area but also provides more reactive active sites. Compared with powder catalysts,this monolithic electrode can achieve intimate contact between the electrocatalyst and the current collector,which will alleviate the problem of pulverization and enable the stable function of the electrode. It can be served as an efficient bi-functional electrocatalyst with an overpotential of 160 mV for HER and 290 mV for OER to produce current densities of 10 mA cm^（-2） in the alkaline medium. And it maintains benign stability after 5,000 cycles,which rivals many recent reported noble-metal free catalysts in 1.0mol L^（-1） KOH solution. Attributed to the easy,scalable methodology and high catalytic efficiency,this work not only offers a promising monolithic catalyst but also inspires us to exploit other inexpensive,highly efficient and self-standing noble metalfree electrocatalysts for scale-up electrochemical water-splitting technology.
基金supported by the National Natural Science Foundation of China(U20A6001,11921002,and 11902292)Zhejiang Province Key Research and Development Project(2021C01183,2020C05004,and 2021C05007-4)the Natural Science Foundation of Zhejiang Province of China(LQ19E030003)。
文摘Signal drift and performance instability of brain-computer interface devices induced by the interface failure between rigid metal electrodes and soft human skin hinder the precise data acquisition of electroencephalogram(EEG).Thus,it is desirable to achieve a robust interface for brain-computer interface devices.Here,a kind of polydopamine methacrylamide-polyacrylamide(PDMA-PAAM)hydrogel is developed.To improve the adhesion,dopamine is introduced into the polyacrylamide hydrogel,through the amino and catechol groups of dopamine in an organic-inorganic interface to build a covalent and non-covalent interaction.A strong attachment and an effective modulus transition system can be formed between the metal electrodes and human skin,so that the peeling force between the PDMAPAAM hydrogel and the porcine skin can reach 22 N m^(-1).In addition,the stable conductivity and long-term operating life of the PDMA-PAAM hydrogel for more than 60 days at room temperature are achieved by adding sodium chloride(NaCl)and glycerol,respectively.The PDMA-PAAM hydrogel membrane fabricated in this work is integrated onto a flexible Au electrode applied in a brain-computer interface.In comparison,the collected EEG signal intensity and waveform are consistent with that of the commercial counterparts.And obviously,the flexible electrode with PDMA-PAAM hydrogel membrane is demonstrated to enable a more stable and userfriendly interface.
