A homogeneous catalyst [Cp*Rh(NH3)(H2O)2]-(3+) has been found for the clean conversion of methanol and water to hydrogen and carbon dioxide. The simple and easily available reaction steps can circumvent the fo...A homogeneous catalyst [Cp*Rh(NH3)(H2O)2]-(3+) has been found for the clean conversion of methanol and water to hydrogen and carbon dioxide. The simple and easily available reaction steps can circumvent the formation of CO, therefore, making it possible to avoid inactivating catalysts and contaminating the hydrogen fuel. Different from conventional reforming method for hydrogen production, no additional alkaline or organic substances are required in this method. Valuable hydrogen can be obtained under ambient pressure at 70 C, corresponding TOF is 83.2 h 1. This is an unprecedented success in reforming methanol to hydrogen. Effects of reaction conditions, such as reaction temperature, initial methanol concentration and the initial p H value of buffer solution on the hydrogen evolution are all systematically investigated. In a certain range, higher reaction temperature will accelerate reaction rate. The slightly acidic condition is conducive to rapid hydrogen production. These findings are of great significance to the present establishment of the carbon-neutral methanol economy.展开更多
Formic acid(FA) dehydrogenation has attracted a lot of attentions since it is a convenient method for H_2 production. In this work, we designed a self-supporting fuel cell system, in which H_2 from FA is supplied in...Formic acid(FA) dehydrogenation has attracted a lot of attentions since it is a convenient method for H_2 production. In this work, we designed a self-supporting fuel cell system, in which H_2 from FA is supplied into the fuel cell, and the exhaust heat from the fuel cell supported the FA dehydrogenation. In order to realize the system, we synthesized a highly active and selective homogeneous catalyst Ir Cp*Cl_2 bpym for FA dehydrogenation. The turnover frequency(TOF) of the catalyst for FA dehydrogenation is as high as7150 h^(-1)at 50°C, and is up to 144,000 h^(-1)at 90°C. The catalyst also shows excellent catalytic stability for FA dehydrogenation after several cycles of test. The conversion ratio of FA can achieve 93.2%, and no carbon monoxide is detected in the evolved gas. Therefore, the evolved gas could be applied in the proton exchange membrane fuel cell(PEMFC) directly. This is a potential technology for hydrogen storage and generation. The power density of the PEMFC driven by the evolved gas could approximate to that using pure hydrogen.展开更多
Single molecule catalysis is very powerful in revealing catalytic mechanism at the single molecule level.But fluorescent molecule is always necessary to take part into the catalysis directly in previous research.In or...Single molecule catalysis is very powerful in revealing catalytic mechanism at the single molecule level.But fluorescent molecule is always necessary to take part into the catalysis directly in previous research.In order to study the single molecule electro-catalysis of non-fluorescent molecule(SMECNFM) on nanocatalyst, we couple the SMECNFM with a single molecule fluorescence reaction. A certain number of fluorescent molecules will be generated and detected when the SMECNFM happens. Through this method, we can detect the electro-oxidation reaction of one HCOONa molecule. The stability of Pt nanocatalyst supported on active carbon is studied at the single molecule level by this method. This paper also provides a general way to make ultra-sensitive sensor, and to study the SMECNFM for the molecules,such as formic acid, hydrogen, oxygen, etc., on single nanoparticle.展开更多
基金financial support granted by Ministry of Science and Technology of the People's Republic of China(Nos.2016YFA0200700 and 2016YFE0105700)the National Natural Science Foundation of China(Nos.21373264 and 21573275)+2 种基金the Natural Science Foundation of Jiangsu Province(No.BK20150362)Suzhou Institute of Nano-tech and Nanobionics(No.Y3AAA11004)Thousand Youth Talents Plan(No.Y3BQA11001)
文摘A homogeneous catalyst [Cp*Rh(NH3)(H2O)2]-(3+) has been found for the clean conversion of methanol and water to hydrogen and carbon dioxide. The simple and easily available reaction steps can circumvent the formation of CO, therefore, making it possible to avoid inactivating catalysts and contaminating the hydrogen fuel. Different from conventional reforming method for hydrogen production, no additional alkaline or organic substances are required in this method. Valuable hydrogen can be obtained under ambient pressure at 70 C, corresponding TOF is 83.2 h 1. This is an unprecedented success in reforming methanol to hydrogen. Effects of reaction conditions, such as reaction temperature, initial methanol concentration and the initial p H value of buffer solution on the hydrogen evolution are all systematically investigated. In a certain range, higher reaction temperature will accelerate reaction rate. The slightly acidic condition is conducive to rapid hydrogen production. These findings are of great significance to the present establishment of the carbon-neutral methanol economy.
基金financial support granted by Ministry of Science and Technology of China(Nos.2016YFE0105700,2016YFA0200700)the National Natural Science Foundation of China(Nos.21373264,21573275)+2 种基金the Natural Science Foundation of Jiangsu Province(No.BK20150362)Suzhou Institute of Nano-tech and Nano-bionics(No.Y3AAA11004)Thousand Youth Talents Plan(No.Y3BQA11001)
文摘Formic acid(FA) dehydrogenation has attracted a lot of attentions since it is a convenient method for H_2 production. In this work, we designed a self-supporting fuel cell system, in which H_2 from FA is supplied into the fuel cell, and the exhaust heat from the fuel cell supported the FA dehydrogenation. In order to realize the system, we synthesized a highly active and selective homogeneous catalyst Ir Cp*Cl_2 bpym for FA dehydrogenation. The turnover frequency(TOF) of the catalyst for FA dehydrogenation is as high as7150 h^(-1)at 50°C, and is up to 144,000 h^(-1)at 90°C. The catalyst also shows excellent catalytic stability for FA dehydrogenation after several cycles of test. The conversion ratio of FA can achieve 93.2%, and no carbon monoxide is detected in the evolved gas. Therefore, the evolved gas could be applied in the proton exchange membrane fuel cell(PEMFC) directly. This is a potential technology for hydrogen storage and generation. The power density of the PEMFC driven by the evolved gas could approximate to that using pure hydrogen.
基金supported by the National Natural Science Foundation of China(Nos.21373264 and 21573275)Suzhou Institute of Nano-tech and Nano-bionics(No.Y3AAA11004)Thousand Youth Talents Plan(No.Y3BQA11001)
文摘Single molecule catalysis is very powerful in revealing catalytic mechanism at the single molecule level.But fluorescent molecule is always necessary to take part into the catalysis directly in previous research.In order to study the single molecule electro-catalysis of non-fluorescent molecule(SMECNFM) on nanocatalyst, we couple the SMECNFM with a single molecule fluorescence reaction. A certain number of fluorescent molecules will be generated and detected when the SMECNFM happens. Through this method, we can detect the electro-oxidation reaction of one HCOONa molecule. The stability of Pt nanocatalyst supported on active carbon is studied at the single molecule level by this method. This paper also provides a general way to make ultra-sensitive sensor, and to study the SMECNFM for the molecules,such as formic acid, hydrogen, oxygen, etc., on single nanoparticle.