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In-Situ FT-IR Investigation Methane to Syngas over of Partial Oxidation of Rh/SiO2 Catalyst 认领 引用 被引量：3
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作者 Tinghua Wu Dongmin Lin +4 位作者 Ying Wu Xiaoping Zhou Qiangu Yan Weizheng Weng Huilin Wan 《Journal of Natural Gas Chemistry》 2007年第3期316-321,共6页
Partial oxidation of methane to syngas （POM） over Rh/SiO2 catalyst was investigated using in-situ FT-IR. When methane interacted with 1.0wt%Rh/SiO2 catalyst, it was dissociated to adsorbed hydrogen and CHx species. ... Partial oxidation of methane to syngas （POM） over Rh/SiO2 catalyst was investigated using in-situ FT-IR. When methane interacted with 1.0wt%Rh/SiO2 catalyst, it was dissociated to adsorbed hydrogen and CHx species. The adsorbed hydrogen atoms were transferred to SiO2 surface by ＂spill-over＂ and reacted with lattice oxygen to form surface -OH species. POM mechanism was investigated over Rh/SiO2 catalyst using in-situ FT-IR. It was found that CO2 was formed before CO could be detected when CH4 and O2 were introduced over the preoxidized Rh/SiO2 catalyst, whereas CO was detected before CO2 was formed over the prereduced Rh/SiO2 catalyst. 展开更多
关键词 partial oxidation syngas Rh/SiO2 catalyst in-situ FT-IR
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载体形貌对Rh/CeO2催化分解N2O的影响 认领 引用
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作者 汪浩然 鲍世东 郑寿荣 《环境化学》 CAS CSCD 北大核心 2026年第5期2115-2124,共10页
N2O是一种重要的温室气体,对其进行催化分解具有重要环境意义.本研究采用水热法分别制备了3种不同形貌的CeO2载体:纳米棒(NR)、纳米立方体(NC)和纳米八面体(NO),然后采用沉淀沉积法制备了Rh/CeO2催化剂.催化性能测试结果表明,... N2O是一种重要的温室气体,对其进行催化分解具有重要环境意义.本研究采用水热法分别制备了3种不同形貌的CeO2载体:纳米棒(NR)、纳米立方体(NC)和纳米八面体(NO),然后采用沉淀沉积法制备了Rh/CeO2催化剂.催化性能测试结果表明,与Rh/CeO2-NC和Rh/CeO2-NO相比,在各种反应条件下,Rh/CeO2-NR的催化性能都相对更好.表征结果显示,Rh/CeO2-NR催化剂含有丰富的氧空位和相对多的本征缺陷位,有利于O中间体转移,且具有合适的Rh0/Rhn+比例,有利于Rh物种和反应物的氧化还原循环,从而增强催化活性. 展开更多
关键词 N2O 直接催化分解 Rh/CeO2催化剂
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CeO2暴露晶面对Rh-CeO2催化剂CO2甲烷化催化性能的影响 认领 引用
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作者 杨红丽 常盼盼 董金诗 《低碳化学与化工》 CAS 北大核心 2026年第6期1-12,共12页
CO2甲烷化是实现“碳中和”的重要化学手段之一,然而开发具有高甲烷(CH4)选择性的催化剂具有一定挑战。采用煅烧法和水热合成法制备了不同微观形貌的CeO2载体,并负载质量分数为0.5%的Rh制备了CeO2暴露晶面不同的Rh-CeO2... CO2甲烷化是实现“碳中和”的重要化学手段之一,然而开发具有高甲烷(CH4)选择性的催化剂具有一定挑战。采用煅烧法和水热合成法制备了不同微观形貌的CeO2载体,并负载质量分数为0.5%的Rh制备了CeO2暴露晶面不同的Rh-CeO2催化剂,通过不同表征方法,系统探究了CeO2暴露晶面对Rh-CeO2催化剂CO2甲烷化催化性能的影响。结果显示,0.5Rh-CeO2-NC(NC表示纳米立方体)催化性能最优,400℃时CH4选择性高达76%,CH4产率为29.19%。CeO2(100)晶面在还原预处理后更容易形成表面氧空位,有利于CO2活化,并且富电子的Rh单原子聚集成纳米颗粒,加强了H2活化,从而促进了CH4生成。原位DRIFTS证实Rh-CeO2催化剂作用下,CO2甲烷化遵循甲酸盐路径与CO路径共存的机制,且两种路径的竞争关系受CeO2暴露晶面调控。 展开更多
关键词 CO2甲烷化 Rh-CeO2催化剂 CeO2暴露晶面
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Hydroformylation of methyl-3-pentenoate over a phosphite ligand modified Rh/SiO_2 catalyst 认领 引用 被引量：2
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作者 Xianming Li Yunjie Ding +3 位作者 Guiping Jiao Jingwei Li Li Yan Hejun Zhu 《Journal of Natural Gas Chemistry》 2008年第4期351-354,共4页
A phosphite ligand modified Rh/SiO2 catalyst has been developed for hydroformylation of internal olefins to linear aldehydes, which showed high activity and regioselectivity and could be separated easily by filtration... A phosphite ligand modified Rh/SiO2 catalyst has been developed for hydroformylation of internal olefins to linear aldehydes, which showed high activity and regioselectivity and could be separated easily by filtration after reaction in an autoclave. Effects of reaction temperature and syngas pressure on the performances of the catalyst in the reaction were also investigated. 展开更多
关键词 Rh/SiO2 phosphite hydroformylation internal olefins linear aldehydes
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Product oriented oxidative bromination of methane over Rh/SiO2catalysts 认领 引用 被引量：4
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作者 Zhen Liu Wensheng Li Xiaoping Zhou 《Journal of Natural Gas Chemistry》 2010年第5期522-529,共8页
Rh/SiO2 was prepared for the oxidative bromination of methane.The catalyst was prepared by calcination at different temperatures and for different times to obtain catalysts with different specific surface areas for th... Rh/SiO2 was prepared for the oxidative bromination of methane.The catalyst was prepared by calcination at different temperatures and for different times to obtain catalysts with different specific surface areas for the purposes of producing either CH3Br or CH3Br and CO.It was found that the catalyst having a low specific surface area(calcined at relatively high temperature)favors the selective oxidation of methane to prepare CH3Br,while the catalyst having a high specific surface area favors the deeper partial oxidation of methane,which is good for CH3Br and CO preparation,The 650 h on stream life-time test revealed that the catalytic performance of the 0.4Rh/SiO2-900-10 catalyst was excellent.Both methane conversion and CH3Br selectivity kept increasing trends during the life-time test.No matter how serious was the Rh leaching during the reaction,the 0.4Rh/SiO2-900-10 catalyst did not deactivate at all. 展开更多
关键词 oxidative bromination of methane methyl bromide Rh/SiO2
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QUANTUM CHEMICAL STUDY ON THE MECHANISM OF PRODUCING OXYGENATES IN FISCHER-TROPSCH SYNTHESIS ON M/SiO_2 (M=Ni, Ru, Rh, Pd) CATALYSTS 认领 引用
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作者 Zheng Ping HAO Tian Wei ZHU Li Dun AN 《Chinese Chemical Letters》 SCIE CAS 1994年第6期511-514,共4页
EHMO calculations and orbital analysis of fragments were performed for the Synthetic reactions of oxygenates in Fischer-Tropsch synthesis using a butterfly model for four different metals (Nim Ru, Rh, Pd)supported on ... EHMO calculations and orbital analysis of fragments were performed for the Synthetic reactions of oxygenates in Fischer-Tropsch synthesis using a butterfly model for four different metals (Nim Ru, Rh, Pd)supported on SiO2 as catalysts. Four processest CO dissociation, coupling of CO and H to produce CHO.insertion of CO to M-CH3; insertion of CH2 to M-CH3 have been calculated. We compared the degree of CO bond activation and the banters of the foregoing processes for these four catalysts, it can be shown that Ni/SiO2 is a methanation catalyst, Ru/SiO2 and Rh/SiO2 can produce C2-oxygenated compound (acetaldehyde), especially Rh/SiO2 is a good catalyst for producing it, and Pd/SiO2 is a methanol Synthesis catalyst. 展开更多
关键词 Pd CATALYSTS Ru SiO Rh Ni
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La2O3助剂对Rh/SiO2催化CO加氢反应性能的影响 认领 引用 被引量：3
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作者 石张平 祁晓岚 +4 位作者 李旭光 李华英 李经球 孔德金 俞俊 《燃料化学学报》 CSCD 北大核心 2020年第4期483-489,I0007,共7页
采用溶胶凝胶法制备了SiO2和La2O3-SiO2载体,再通过浸渍法分别引入Rh-La和Rh组分,研究考察了La引入方式对Rh/SiO2催化CO加氢反应性能的影响。结果表明,La的添加有利于提高Rh的分散度,促进Rh+中心数的增加,有效地抑制产物中CO2的生成,提... 采用溶胶凝胶法制备了SiO2和La2O3-SiO2载体,再通过浸渍法分别引入Rh-La和Rh组分,研究考察了La引入方式对Rh/SiO2催化CO加氢反应性能的影响。结果表明,La的添加有利于提高Rh的分散度,促进Rh+中心数的增加,有效地抑制产物中CO2的生成,提高含氧化合物选择性。此外,La的引入方式会影响La与Rh间的相互作用强弱,Rh和La共浸渍制得的2Rh-5La2O3/SiO2催化剂中Rh-La相互作用较强,削弱的Rh-CO键有利于反应过程中CO的插入反应,使得产物以C2+含氧化合物为主。而La以助剂形式掺入SiO2制得的2Rh/5La2O3-SiO2催化剂具有较弱的La-Rh相互作用,其产物则以甲醇、乙醇等低碳醇为主。 展开更多
关键词 La2O3助剂 Rh/SiO2催化剂 CO加氢 C2含氧化合物
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金属粒径对锚合膦配体修饰的Rh/SiO_2催化剂氢甲酰化性能的影响 认领 引用 被引量：3
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作者 刘佳 严丽 +1 位作者 姜淼 丁云杰 《高等学校化学学报》 SCIE EI CAS CSCD 北大核心 2016年第1期114-120,共7页
在相同Rh担载量和P/Rh摩尔比的条件下,使用壳型催化剂制备技术制备了具有不同Rh粒径的锚合膦配体修饰的Rh/SiO_2催化剂,以乙烯氢甲酰化反应作为探针反应考察了催化剂的反应性能.结果表明,Rh粒径直接影响催化剂的催化性能:Rh粒径越小,催... 在相同Rh担载量和P/Rh摩尔比的条件下,使用壳型催化剂制备技术制备了具有不同Rh粒径的锚合膦配体修饰的Rh/SiO_2催化剂,以乙烯氢甲酰化反应作为探针反应考察了催化剂的反应性能.结果表明,Rh粒径直接影响催化剂的催化性能:Rh粒径越小,催化剂活性越高,但诱导期越长.通过H2化学吸附、透射电子显微镜、N_2吸附-脱附等温线、原位红外光谱和固体31P核磁共振技术对催化剂进行了表征,结果表明,随着Rh粒径的减小,活性物种铑膦配合物增多,但有效载体面积上的Rh颗粒浓度降低,使膦需要更多的时间和Rh配位形成配合物,从而导致诱导期增长. 展开更多
关键词 锚合膦配体 Rh/SiO2 壳型催化剂 乙烯 氢甲酰化反应
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Effect of SiO2 addition on NH4HSO4 decomposition and SO2 poisoning over V2O5-MoO3/TiO2-CeO2 catalyst 认领 引用 被引量：11
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作者 Chengqiang Zheng Teng Cheng +2 位作者 Linjun Yang Hao Wu Hongmei Fan 《Journal of Environmental Sciences》 SCIE EI CAS CSCD 2020年第5期279-291,共13页
The deposition of NH4 HSO4 and the poisoning effect of SO2 on SCR catalyst are the main obstacles that restrict the industrial application of CeO2-doped SCR catalysts.In this work,deposited NH4 HSO4 decomposition beha... The deposition of NH4 HSO4 and the poisoning effect of SO2 on SCR catalyst are the main obstacles that restrict the industrial application of CeO2-doped SCR catalysts.In this work,deposited NH4 HSO4 decomposition behavior and SO2 poisoning over V2 O5-MoO3/TiO2 catalysts modified with CeO2 and SiO2 were investigated.By the means of characterization analysis,it was found that the addition of SiO2 into VMo/Ti-Ce had an impact on the interaction existed between catalyst surface atoms and NH4 HSO4.Temperatureprogrammed methods and in situ diffused reflectance infrared Fourier transform spectroscopy(DRIFTS)experiments indicated that the doping of SiO2 promoted the decomposition of deposited NH4 HSO4 on VMo/Ti-Ce catalyst surface by reducing the thermal stability of NH4 HSO4 and enhancing the NH4 HSO4 reactivity with NO in low temperature.And this improvement may be the reason for the better catalytic activity than VMo/Ti-Ce in the case of NH4 HSO4 deposition.Accompanied with cerium sulfate species generated over catalyst surface,the conversion of SO2 to SO3 was inhibited in SiCe mixed catalyst.The addition of SiO2 could promote the decomposition of cerium sulfate,which may be a potential strategy to enhance the resistance of SO2 poisoning over CeO2-modifed catalysts. 展开更多
关键词 CeO2-doped SCR catalyst SiO2 addition NH4HSO4 decomposition SO2 poisoning Cerium sulfate
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Regulating local coordination environment of rhodium single atoms in Rh/CeO2 catalysts for N2O decomposition 认领 引用 被引量：9
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作者 Shaohua Xie Daekun Kim +2 位作者 Kailong Ye Laurene Tetard Fudong Liu 《Journal of Rare Earths》 SCIE EI CAS CSCD 2023年第6期941-951,I0005,共11页
Rh single atom catalysts(SACs)have been insensitively investigated recently due to the maximum utilization efficiency of Rh,one of the most expensive precious metals.Although great efforts have been made in the develo... Rh single atom catalysts(SACs)have been insensitively investigated recently due to the maximum utilization efficiency of Rh,one of the most expensive precious metals.Although great efforts have been made in the development and application of Rh SACs,there are few reports on the precise control of the local coordination environment of Rh single sites on CeO2 and their catalytic performance for N2O decomposition.Herein,Rh/CeO2 catalysts with different Rh-O coordination numbers(CNs)were successfully prepared using different CeO2 supports and a simple incipient wetness impregnation(IWI)method.It is observed that the Rh/CeO2 catalyst with slightly higher CN of Rh-O(Rh/CeO2-H)prepared from CeO2 shows much higher N2O decomposition activity than the catalyst with lower CN of Rh-O(Rh/CeO2-L)obtained from Ce(OH)x.The Rh species within Rh/CeO2-H are found to be more reactive than those within Rh/CeO2-L,which can better facilitate the O2desorption once formed during N2O deco mposition.In additio n,more surface oxygen vacancies are present on Rh/CeO2-H than on Rh/CeO2-L,well explaining the superior N2O adsorption and activation capability on the former catalyst.It is concluded that more abundant oxygen vacancies and reactive Rh single atom sites with slightly higher CN of Rh-O and significantly higher reducibility altogether contribute to the superior N2O decomposition activity on the Rh/CeO2-H catalyst. 展开更多
关键词 Rh single-atom catalyst Coordination environment N2O decomposition Oxygen vacancy O2desorption Rare earths
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The effect of ethanol on the performance of CrO_x/SiO_2 catalysts during propane dehydrogenation 认领 引用 被引量：5
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作者 李利娜 朱文良 +6 位作者 石磊 刘勇 刘红超 倪友明 刘世平 周慧 刘中民 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2016年第3期359-366,共8页
The effects of ethanol vapor pretreatment on the performance of CrOx/SiO2 catalysts during the dehydrogenation of propane to propylene were studied with and without the presence of CO2.The catalyst pretreated with eth... The effects of ethanol vapor pretreatment on the performance of CrOx/SiO2 catalysts during the dehydrogenation of propane to propylene were studied with and without the presence of CO2.The catalyst pretreated with ethanol vapor exhibited better catalytic activity than the pristine CrOx/SiO2,generating 41.4% propane conversion and 84.8% propylene selectivity.The various catalyst samples prepared were characterized by X-ray diffraction,transmission electron microscopy,temperature-programmed reduction,X-ray photoelectron spectroscopy and reflectance UV-Vis spectroscopy.The data show that coordinative Cr^3＋ species represent the active sites during the dehydrogenation of propane and that these species serve as precursors for the generation of Cr^3＋.Cr^3＋ is reduced during the reaction,leading to a decrease in catalytic activity.Following ethanol vapor pretreatment,the reduced CrOx in the catalyst is readily re-oxidized to Cr^6＋ by CO2.The pretreated catalyst thus exhibits high activity during the propane dehydrogenation reaction by maintaining the active Cr^3＋ states. 展开更多
关键词 Propane Dehydrogenation CrOx/SiO2 catalyst Ethanol vapor pretreatment Carbon dioxide
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单分散SiO_2的焙烧温度对Rh基催化剂上CO加氢反应性能的影响 认领 引用 被引量：3
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作者 俞俊 毛东森 +2 位作者 郭强胜 韩璐蓬 卢冠忠 《物理化学学报》 SCIE CAS CSCD 北大核心 2012年第3期667-673,共7页
在比较了分别以商业SiO2和采用Sto?ber法制备的单分散SiO2为载体的Rh-Mn-Li/SiO2催化剂催化CO加氢反应性能的基础上,进一步调变了Stober法制备SiO2时的焙烧温度,并考察了其对Rh-Mn-Li/SiO2催化CO加氢性能的影响.利用N2吸附-脱附、傅... 在比较了分别以商业SiO2和采用Sto?ber法制备的单分散SiO2为载体的Rh-Mn-Li/SiO2催化剂催化CO加氢反应性能的基础上,进一步调变了Stober法制备SiO2时的焙烧温度,并考察了其对Rh-Mn-Li/SiO2催化CO加氢性能的影响.利用N2吸附-脱附、傅里叶变换红外(FTIR)光谱、H2程序升温还原(H2-TPR)、程序升温表面反应(TPSR)等方法对载体及催化剂的物理化学性能进行了表征.结果表明:不同温度焙烧的载体表面具有不同的Si―OH数量,从而影响金属的分散状态及Rh和Mn之间的相互作用.载体表面较多的羟基有利于Rh的分散和CO的吸附,从而增强催化剂的反应活性.载体表面适当数量的羟基能够得到适中的Rh与Mn之间的相互作用,使催化剂具有合适的CO解离能力,有利于CHx的CO插入反应,从而提高了C2含氧化合物的选择性. 展开更多
关键词 Rh-Mn-Li/SiO2 CO加氢 C2含氧化合物 焙烧温度
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High Activity and Selectivity of Cu/SiO_2 Catalyst for the Direct Synthesis of Indole 认领 引用 被引量：3
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作者 Lei SHI Jun Ming SUN +2 位作者 Xin Ping WANG Xan Yun SU Tian Xi CAI 《Chinese Chemical Letters》 SCIE CAS 2002年第3期211-212,共2页
Copper supported over silica exhibited very high activity and selectivity for the direct synthesis of indole at atmospheric pressure. Under the reaction temperature of 325C,the yield of indole could obtain 88%.
关键词 Cu/SiO2 catalyst direct synthesis of indole aniline ethylene glycol.
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浸渍溶剂对Rh-Mn-Li/SiO_2催化剂CO加氢性能的影响 认领 引用 被引量：3
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作者 江大好 丁云杰 +5 位作者 潘振栋 李显明 焦桂萍 李经伟 陈维苗 罗洪原 《天然气化工—C1化学与化工》 北大核心 2007年第5期5-8,共4页
采用CO加氢反应、CO-TPD、TPSR和XPS等技术,考察了水、甲醇、乙醇和异丙醇等浸渍溶剂对Rh-Mn-Li/S iO2催化剂CO加氢性能的影响。结果表明,以乙醇为浸渍溶剂的催化剂表现出最高的C2含氧化合物时空收率(YC2-oxy)和C2含氧化合物选择性(SC2-... 采用CO加氢反应、CO-TPD、TPSR和XPS等技术,考察了水、甲醇、乙醇和异丙醇等浸渍溶剂对Rh-Mn-Li/S iO2催化剂CO加氢性能的影响。结果表明,以乙醇为浸渍溶剂的催化剂表现出最高的C2含氧化合物时空收率(YC2-oxy)和C2含氧化合物选择性(SC2-oxy),分别达686.1 g/(kg-cat.h)和73.8%;以甲醇和异丙醇为浸渍溶剂的催化剂上YC2-oxy也较高,但是SC2-oxy都比前者低;水溶液浸渍制备的催化剂有着较高的SC2-oxy,但是其YC2-oxy较低。以醇类为浸渍溶剂的催化剂的高活性与金属活性组分在催化剂表面富集而导致的更多活性中心的形成有关。催化剂表面非解离的CO比率增加有利于C2含氧化合物选择性的提高。 展开更多
关键词 渍溶剂 Rh-Mn-Li/SiO2催化剂 C2含氧化合物 CO加氢
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Effects of operating parameters on oxidative coupling of methane over Na-W-Mn/SiO_2 catalyst at elevated pressures 认领 引用 被引量：2
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作者 Jafar Sadeghzadeh Ahari Mohammad Taghi Sadeghi Saeed Zarrinpashne 《Journal of Natural Gas Chemistry》 CSCD 2011年第2期204-213,共10页
The effects of operating parameters on oxidative coupling of methane （OCM） over Na-W-Mn/SiO2 catalyst have been studied at elevated pressures of 0.2, 0.3 and 0.4 MPa under low gaseous hourly space velocity （GHSV） ... The effects of operating parameters on oxidative coupling of methane （OCM） over Na-W-Mn/SiO2 catalyst have been studied at elevated pressures of 0.2, 0.3 and 0.4 MPa under low gaseous hourly space velocity （GHSV） and low temperature conditions. Experimental results show that when the operating pressure is increased, C2＋ yield slightly decreases, while the maximum ratio of ethylene to ethane remains unchanged. Moreover, it has been found empirically that increase of pressure does not affect the catalyst behavior permanently, the catalyst recovers its original low pressure performance without hysteresis behavior by reducing the pressure. Under the investigated conditions, when oxygen is completely consumed, the increase of GHSV leads to improvement in C2 selectivity, while C3＋ and COx selectivities decrease slightly. The C2＋ selectivity increases by increase of nitrogen diluent in the feed, but the C3＋ hydrocarbons selectivities decrease with increase of nitrogen since it is possible that further dilution at high pressure may reduce the probability of collision between CH3 and C2＋ hydrocarbons. During the stability test at high pressure, the catalyst performance remains unchanged throughout the 20 h running. The fresh and used catalysts were characterized using XRD, SEM and N2 adsorption-desorption methods. It was found that the phase transformation of the support from α-cristobalite to tridymite and quartz does not have obvious effect on catalyst performance at high pressure. 展开更多
关键词 operating parameters oxidative coupling of methane Na-W-Mn/SiO2 catalyst elevated pressure
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Rh/SiO_2催化剂上双环戊二烯氢甲酰化 认领 引用 被引量：3
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作者 马昱博 高志贤 吾满江.艾力 《工业催化》 CAS 2012年第11期52-56,共5页
采用浸渍法制备了SiO2低负载量的铑催化剂Rh/SiO2。研究以三苯基膦为配体的Rh/SiO2催化剂对双环戊二烯氢甲酰化合成三环癸烷不饱和单醛的催化性能及其影响因素。结果表明,Rh/SiO2催化剂对双环戊二烯氢甲酰化具有良好的催化作用,双环戊... 采用浸渍法制备了SiO2低负载量的铑催化剂Rh/SiO2。研究以三苯基膦为配体的Rh/SiO2催化剂对双环戊二烯氢甲酰化合成三环癸烷不饱和单醛的催化性能及其影响因素。结果表明,Rh/SiO2催化剂对双环戊二烯氢甲酰化具有良好的催化作用,双环戊二烯合成三环癸烷不饱和单醛选择性超过99%。双环戊二烯氢甲酰化过程与催化剂用量、三苯基膦浓度、反应压力和反应温度有关。反应过程中存在一定诱导期,随着压力增加,诱导期逐渐缩短;增加催化剂用量和三苯基膦浓度有利于提高双环戊二烯转化率和三环癸烷不饱和单醛收率;升高温度虽然有利于双环戊二烯转化,却降低了三环癸烷不饱和单醛选择性。当催化剂与双环戊二烯质量比为1∶25、三苯基膦浓度10.0 g.L-1、负载铑质量分数1‰、反应温度110℃、反应压力3.0 MPa和反应时间240 min时,双环戊二烯转化率超过99%,三环癸烷不饱和单醛选择性超过99%。 展开更多
关键词 催化化学 Rh SiO2催化剂 双环戊二烯 三环癸烷不饱和单醛 氢甲酰化 诱导期
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Quaternary phosphonium polymer-supported dual-ionically bound[Rh(CO)I3]2-catalyst for heterogeneous ethanol carbonylation 认领 引用 被引量：1
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作者 Zhou Ren Yang Liu +4 位作者 Yuan Lyu Xiangen Song Changyong Zheng Zheng Jiang Yunjie Ding 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2021年第4期606-617,共12页
A single-Rh-site catalyst(Rh-TPISP)that was ionically-embedded on a P(V)quaternary phosphonium porous polymer was evaluated for heterogeneous ethanol carbonylation.The[Rh(CO)I3]2-unit was proposed to be the acti... A single-Rh-site catalyst(Rh-TPISP)that was ionically-embedded on a P(V)quaternary phosphonium porous polymer was evaluated for heterogeneous ethanol carbonylation.The[Rh(CO)I3]2-unit was proposed to be the active center of Rh-TPISP for the carbonylation reaction based on detailed Rh L3-edge X-ray absorption near edge structure(XANES),X-ray photoelectron spectroscopy(XPS),and Rh extended X-ray absorption fine structure(EXAFS)analyses.As the highlight of this study,Rh-TPISP displayed distinctly higher activity for heterogeneous ethanol carbonylation than the reported catalytic systems in which[Rh(CO)2I2]-is the traditional active center.A TOF of 350 h-1was obtained for the reaction over[Rh(CO)I3]2-,with>95%propionyl selectivity at 3.5 MPa and 468 K.No deactivation was detected during a near 1000 h running test.The more electron-rich Rh center was thought to be crucial for explaining the superior activity and selectivity of Rh-TPISP,and the formation of two ionic bonds between[Rh(CO)I3]2-and the cationic P(V)framework([P]+)of the polymer was suggested to play a key role in firmly immobilizing the active species to prevent Rh leaching. 展开更多
关键词 Heterogeneous ethanol carbonylation Single-site catalyst Carbonylation active center [Rh(CO)I3]2- Ultrastable dual-ionically bound immobilization Porous ionic polymer
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Atomic Dispersion of Rh on Interconnected Mo2C Nanosheet Network Intimately Embedded in 3D NixMoOy Nanorod Arrays for pH-Universal Hydrogen Evolution 认领 引用 被引量：1
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作者 Thi Luu Luyen Doan Dinh Chuong Nguyen +5 位作者 Patrick M.Bacirhonde Ahmed S.Yasin Abdelrahman I.Rezk Nelson Y.Dzade Cheol Sang Kim Chan Hee Park 《Energy & Environmental Materials》 SCIE EI CAS CSCD 2023年第5期236-250,共15页
Herein,a simple synthetic approach is employed for the atomic dispersion of Rh atoms(Rh SAs)over the surface of interconnected Mo2C nanosheets intimately embedded in a three-dimensional NixMoOynanorod arrays(... Herein,a simple synthetic approach is employed for the atomic dispersion of Rh atoms(Rh SAs)over the surface of interconnected Mo2C nanosheets intimately embedded in a three-dimensional NixMoOynanorod arrays(NixMoOyNRs)framework;we found that the introduction of both isolated Rh SAs and NixMoOyNRs adjusts the electrocatalytic function of the host Mo2C toward the direction of being an advanced and highly stable electrocatalyst for efficient hydrogen evolution at pH-universal conditions.As a result,the proposed catalyst outperforms most recently reported transition metal-based catalysts,and its performance even rivals that of commercial Pt/C,as demonstrated by its ultralow overpotentials of 31.7,109.7,and 95.4 mV at a current density of 10 mA cm-2,along with its small Tafel slopes of 42.4,51.2,and 46.8 mV dec-1in acidic,neutral,and alkaline conditions,respectively.In addition,the catalyst shows remarkable long-term stability over all pH values with good maintenance of its catalytic activity and structural characteristics after continuous operation. 展开更多
关键词 hydrogen evolution reaction Mo2C nanosheets NixMoOynanorod arrays pH-universal catalyst single Rh atoms
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Synthesis of Methyl Glycolate by Hydrogenation of Dimethyl Oxalate over Cu-Ag/SiO_2 Catalyst 认领 引用 被引量：26
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作者 Baowei Wang Qian Xu Hua Song Genhui Xu 《Journal of Natural Gas Chemistry》 2007年第1期78-80,共3页
Methyl glycolate is a good solvent and can be used as feedstock for the synthesis of some important organic chemicals. Catalytic hydrogenation of dimethyl oxalate （DMO） over copper-silver catalyst supported on silic... Methyl glycolate is a good solvent and can be used as feedstock for the synthesis of some important organic chemicals. Catalytic hydrogenation of dimethyl oxalate （DMO） over copper-silver catalyst supported on silica was studied. The Cu-Ag/SiO2 catalyst supported on silica sol was prepared by homogeneous deposition-precipitation of the mixture of aqueous euprammonia complex and silica sol. The proper active temperature of Cu-Ag/SiO2 catalyst for hydrogenation of DMO was 523-623 K. The most preferable reaction conditions for methyl glycolate （MG） were optimized： temperature at 468-478 K, 40-60 mesh catalyst diameter, H2/DMO ratio 40, and 1.0 h^-1 of LHSV. 展开更多
关键词 dimethyl oxalate methyl glycolate ethylene glycol hydrogenation Cu-Ag/SiO2 catalyst
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Rh/SiO_2催化剂上甲烷部分氧化制合成气反应 认领 引用 被引量：3
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作者 吴廷华 严前古 +5 位作者 李少斌 钟依均 牛振江 朱明乔 李则林 万惠霖 《催化学报》 2003年第6期407-413,共7页
利用程序升温脱附、程序升温还原、程序升温表面反应、程序升温反应和化学捕获反应等手段 ,对Rh/SiO2 催化剂上甲烷部分氧化制合成气反应进行了研究 .结果表明 ,Rh/SiO2 催化剂上甲烷部分氧化制合成气机理属于热解 氧化反应机理 .甲烷... 利用程序升温脱附、程序升温还原、程序升温表面反应、程序升温反应和化学捕获反应等手段 ,对Rh/SiO2 催化剂上甲烷部分氧化制合成气反应进行了研究 .结果表明 ,Rh/SiO2 催化剂上甲烷部分氧化制合成气机理属于热解 氧化反应机理 .甲烷首先在催化剂上发生解离吸附 ,产生具有不同H/C比的化学吸附物种CHx(x =1～ 3) .其中 ,具有较高H/C比的CHx 可能是甲烷部分氧化反应的活性物种 ,而具有较低H/C比的CHx 可能是催化剂上积碳并导致催化剂失活的来源 .活性物种CHx在活性氧物种的作用下 ,生成含氧中间体物种CHxO或继续脱氢 .含氧中间体物种进一步分解 ,即生成CO和H2 ;CO2 也可由CHx 展开更多
关键词 Rh/SiO2催化剂 甲烷 部分氧化 合成气 制备 氧化硅 铑 化学捕获反应
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