Aqueous precipitation and deposition-precipitation method were used to prepare CeO2 supports and Au/CeO2 catalysts, respectively. The effect of preparation condition of support on the catalyst activity was investigate...Aqueous precipitation and deposition-precipitation method were used to prepare CeO2 supports and Au/CeO2 catalysts, respectively. The effect of preparation condition of support on the catalyst activity was investigated. The catalytic combustion of HCHO was considered as the probe reaction for comparing the catalyst activity. The BET, X-ray diffraction, X-ray photoelectron spectroscopy （XPS）, and reduction （TPR） were carried out to analyze the influence factor on the catalysts activity. The results showed that the addition of dispersant and use of microwave in the support preparation procedure could be beneficial for enhancing the interaction of supports and gold species and thus improved the catalytic activity. The total conversion temperature for HCHO was 146 ℃ over AC400. With the modification during supports preparation process, the catalytic activity increased with total conversion temperature decreasing to 98 ℃. The results of XPS indicated that Au^0 and Au^＋1 species coexisted in these catalysts and the activity of catalyst correlated with Au^＋1/Au^0 ratio. Temperature-programmed reduction results demonstrated that the reduction peak appeared between 100-170 ℃ with the inducing of gold. The dependence of activity on the reduction peak temperature implied that ionic gold was catalytic activity component for HCHO oxidation.展开更多
The preferential oxidation of CO （CO‐PROX） is a hot topic because of its importance in pro‐ton‐exchange membrane fuel cells （PEMFCs）. Au catalysts are highly active in CO oxidation. Howev‐er, their activities ...The preferential oxidation of CO （CO‐PROX） is a hot topic because of its importance in pro‐ton‐exchange membrane fuel cells （PEMFCs）. Au catalysts are highly active in CO oxidation. Howev‐er, their activities still need to be improved at the PEMFC operating temperatures of 80–120 ＆#176;C. In the present study, Au nanoparticles of average size 2.6 nm supported on ceria‐modified Al2O3 were synthesized and characterized using powder X‐ray diffraction, nitrogen physisorption, transmission electron and scanning transmission electron microscopies, temperature‐programmed hydrogen reduction （H2‐TPR）, Raman spectroscopy, and in situ diffuse‐reflectance infrared Fourier‐transform spectroscopy. Highly dispersed Au nanoparticles and strong structures formed by Au–support in‐teractions were the main active species on the ceria surface. The Raman and H2‐TPR results show that the improved catalytic performance of the Au catalysts can be attributed to enhanced strong metal–support interactions and the reducibility caused by ceria doping. The formation of oxygen vacancies on the catalysts increased their activities in CO‐PROX. The synthesized Au catalysts gave excellent catalytic performances with high CO conversions （＆gt;97%） and CO2 selectivities （＆gt;50%） in the temperature range 80–150 ＆#176;C.展开更多
Hydrothermal alteration with bleaching of host rocks is the most important prospecting indicator for gold deposits in the Jiangnan Orogen Belt.The alteration has been identified as pre-ore carbonate(siderite)-sericiti...Hydrothermal alteration with bleaching of host rocks is the most important prospecting indicator for gold deposits in the Jiangnan Orogen Belt.The alteration has been identified as pre-ore carbonate(siderite)-sericitization and the Fe of siderite in the alteration zone is derived from the host rocks rather than fluids.In addition,such alteration decreases in intensity and width with depth and gold mineralization also occur in the non-bleached rocks,casting doubt on the reliability of the prospecting indicator.Detailed petrographic work and SEM analysis on the Wangu deposit indicate that there are two types of siderites,i.e.,Sd1 and Sd2.Among them,Sd1 grains are relatively small and distributed along the planes of unaltered host rocks,while Sd2 grains,only occurring in the altered slates,are commonly larger.Both types of siderites were altered by auriferous fluids,producing porous cores and minerals such as pyrite,quartz,and ankerite.Compared with unaltered parts,the altered parts have lower Fe,but higher U,Pb,and REE.In addition,Sd1 and Sd2 are similar in Mn,Na,V,and Sr concentrations but different in Fe and Mg.The occurrence and geochemical compositions of both siderites indicate that Sd1 could be transformed into Sd2 by pre-mineralization alteration through dissolution-reprecipitation.Chlorite is another important Fe-bearing mineral in the host rocks,and EPMA analysis suggests that it is ripidolite with relatively high Fe contents.Consequently,chlorite can also provide Fe to form the pre-ore carbonate(siderite)-sericitization.Geochemical modeling demonstrates that both ripidolite and siderite can result in sulfidation and therefore gold precipitation.As a result,this study demonstrates that pre-ore alteration with characterized bleaching is not a prerequisite for gold mineralization despite of its prominent features.Due to the presence of Fe-bearing Sd1 and chlorite,gold mineralization could still occur through sulfidation in the unaltered rocks.展开更多
基金the National Natural Science Foundation of China (20563003)Natural Science Foundation of Inner Mongolia (200508010203)
文摘Aqueous precipitation and deposition-precipitation method were used to prepare CeO2 supports and Au/CeO2 catalysts, respectively. The effect of preparation condition of support on the catalyst activity was investigated. The catalytic combustion of HCHO was considered as the probe reaction for comparing the catalyst activity. The BET, X-ray diffraction, X-ray photoelectron spectroscopy （XPS）, and reduction （TPR） were carried out to analyze the influence factor on the catalysts activity. The results showed that the addition of dispersant and use of microwave in the support preparation procedure could be beneficial for enhancing the interaction of supports and gold species and thus improved the catalytic activity. The total conversion temperature for HCHO was 146 ℃ over AC400. With the modification during supports preparation process, the catalytic activity increased with total conversion temperature decreasing to 98 ℃. The results of XPS indicated that Au^0 and Au^＋1 species coexisted in these catalysts and the activity of catalyst correlated with Au^＋1/Au^0 ratio. Temperature-programmed reduction results demonstrated that the reduction peak appeared between 100-170 ℃ with the inducing of gold. The dependence of activity on the reduction peak temperature implied that ionic gold was catalytic activity component for HCHO oxidation.
基金supported by the National Basic Research Program of China (973 Program, 2013CB934104)the National Natural Science Founda-tion of China (21225312, U1303192)~~
文摘The preferential oxidation of CO （CO‐PROX） is a hot topic because of its importance in pro‐ton‐exchange membrane fuel cells （PEMFCs）. Au catalysts are highly active in CO oxidation. Howev‐er, their activities still need to be improved at the PEMFC operating temperatures of 80–120 ＆#176;C. In the present study, Au nanoparticles of average size 2.6 nm supported on ceria‐modified Al2O3 were synthesized and characterized using powder X‐ray diffraction, nitrogen physisorption, transmission electron and scanning transmission electron microscopies, temperature‐programmed hydrogen reduction （H2‐TPR）, Raman spectroscopy, and in situ diffuse‐reflectance infrared Fourier‐transform spectroscopy. Highly dispersed Au nanoparticles and strong structures formed by Au–support in‐teractions were the main active species on the ceria surface. The Raman and H2‐TPR results show that the improved catalytic performance of the Au catalysts can be attributed to enhanced strong metal–support interactions and the reducibility caused by ceria doping. The formation of oxygen vacancies on the catalysts increased their activities in CO‐PROX. The synthesized Au catalysts gave excellent catalytic performances with high CO conversions （＆gt;97%） and CO2 selectivities （＆gt;50%） in the temperature range 80–150 ＆#176;C.
基金co-founded by the National Natural Science Foundation of China(42002090,41930428)National Key Research and Development Program of China(No.2018YFC0604200)+3 种基金Open Research Fund Program of State Key Laboratory of Nuclear Resources and Environment,East China University of Technology(No.NRE1915)Open Research Fund Program of Jiangxi Engineering Laboratory on Radioactive Geoscience and Big Data Technology(JELRGBDT202006)International Geoscience Programme(IGCP675)Jiangxi province graduate student innovation special fund project(YC2019-S271,DHYC-202001)。
文摘Hydrothermal alteration with bleaching of host rocks is the most important prospecting indicator for gold deposits in the Jiangnan Orogen Belt.The alteration has been identified as pre-ore carbonate(siderite)-sericitization and the Fe of siderite in the alteration zone is derived from the host rocks rather than fluids.In addition,such alteration decreases in intensity and width with depth and gold mineralization also occur in the non-bleached rocks,casting doubt on the reliability of the prospecting indicator.Detailed petrographic work and SEM analysis on the Wangu deposit indicate that there are two types of siderites,i.e.,Sd1 and Sd2.Among them,Sd1 grains are relatively small and distributed along the planes of unaltered host rocks,while Sd2 grains,only occurring in the altered slates,are commonly larger.Both types of siderites were altered by auriferous fluids,producing porous cores and minerals such as pyrite,quartz,and ankerite.Compared with unaltered parts,the altered parts have lower Fe,but higher U,Pb,and REE.In addition,Sd1 and Sd2 are similar in Mn,Na,V,and Sr concentrations but different in Fe and Mg.The occurrence and geochemical compositions of both siderites indicate that Sd1 could be transformed into Sd2 by pre-mineralization alteration through dissolution-reprecipitation.Chlorite is another important Fe-bearing mineral in the host rocks,and EPMA analysis suggests that it is ripidolite with relatively high Fe contents.Consequently,chlorite can also provide Fe to form the pre-ore carbonate(siderite)-sericitization.Geochemical modeling demonstrates that both ripidolite and siderite can result in sulfidation and therefore gold precipitation.As a result,this study demonstrates that pre-ore alteration with characterized bleaching is not a prerequisite for gold mineralization despite of its prominent features.Due to the presence of Fe-bearing Sd1 and chlorite,gold mineralization could still occur through sulfidation in the unaltered rocks.
