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Grain boundary engineering of CeO2 induced electron redistribution for dimethyl carbonate synthesis from CO2 认领 引用
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作者 Guoqiang Hou Di Xu +3 位作者 Haifeng Fan Yangyang Li Siyi Huang Mingyue Ding 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2026年第1期316-329,共14页
Direct synthesis of dimethyl carbonate(DMC)from CO2 is critical for achieving carbon neutrality,yet the sluggish formation and conversion of the key*CH₃OCOO intermediate-due to the difficulty of C-O coupling-limit ... Direct synthesis of dimethyl carbonate(DMC)from CO2 is critical for achieving carbon neutrality,yet the sluggish formation and conversion of the key*CH₃OCOO intermediate-due to the difficulty of C-O coupling-limit high DMC yields.Herein,we developed a boric acid-assisted recrystallization strategy to fabricate grain-boundary-rich CeO2 hollow nanospheres,which serve as an efficient catalyst for CO2 to DMC synthesis.The introduction of grain-boundary(GBs)induced the electron redistribution,which led a decrease in the electron density of bulk Ce ions and created a localized electron-rich region at homogeneous interface.This unique electronic landscape promoted reactive methoxy formation and stronger CO2 adsorption,thereby enabling more efficient coupling of*CH3O and*CO2 to form the*CH3OCOO.Concurrently,the enhanced CO2 adsorption facilitated the dissociation of*CH3OCOO and subsequent DMC formation.As a result,the 4%BCeO2-GBs achieved an advantageous DMC yield of 19.8 mmol/g.In the assistance of dehydrating agent,the catalyst delivered a remarkable 264.2 mmol/g DMC yield and 7.12%methanol conversion,which was 32 times higher than commercial CeO2.This study elucidated the intrinsic mechanisms governing*CH3OCOO intermediate behavior and offers valuable guidance for CO2 converting into high-value organic chemicals. 展开更多
关键词 Dimethyl carbonate synthesis CeO2 catalyst Grain boundary engineering Electron redistribution Reaction intermediates
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Theoretical Study of Dehydrogenation Reaction Mechanism on Cu10/TiO2,Au10/TiO2,Au8Cu2/TiO2,or Cu1/Au8Cu2/TiO2Surfaces 认领 引用
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作者 Hongwei Li Ruimin Wang +2 位作者 Caifang Han Bo Ren Hongjun Fan 《Chinese Journal of Chemical Physics》 SCIE EI CAS CSCD 2026年第2期225-232,I0069-I0071,I0170,共8页
Comprehensive analysis of the connection be-tween surface metal species and the mechanism of hydrogen(H2)generation on TiO2provides important new information for the develop-ment of more effective catalysts for ... Comprehensive analysis of the connection be-tween surface metal species and the mechanism of hydrogen(H2)generation on TiO2provides important new information for the develop-ment of more effective catalysts for H2 produc-tion.We have systematically investigated the mechanism of catalytic H2 generation on the Cu10/TiO2,Au10/TiO2,Au8Cu2/TiO2and Cu1/Au8Cu2/TiO2surfaces using density func-tional theory.Our results demonstrate an O-Hδ+···Hδ−-M type transition state for H2 production,and the Au8Cu2(0.54 eV)bimetal-lic cluster catalyst exhibits more activity in comparison to the Cu10(0.63 eV)and Au10(0.88 eV)cluster catalysts on the TiO2surface.On the Cu1/Au8Cu2/TiO2surface,we found that Au8Cu2clusters act as electron donors,while Cu single atom acts as an electron acceptor.Therefore,the Au8Cu2bimetallic catalyst has a low energy barrier(0.58 eV)in the reductive reaction of H2 production in water,but Cu single atom as the catalytic center has a higher en-ergy barrier(1.49 eV).This implies that bimetallic catalysts may be able to catalyze the wa-ter dehydrogenation reaction more successfully,which would be important knowledge for comprehending and refining the photocatalytic H2 generation process. 展开更多
关键词 TiO2surface Metal cluster Dehydrogenation Cu Au Bimetallic catalyst Den-sity functional theory
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Preparation of Au/CeO_2 catalyst and its catalytic performance for HCHO oxidation 认领 引用 被引量：8
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作者 贾美林 白海锋 +2 位作者 照日格图 沈岳年 李彦锋 《Journal of Rare Earths》 SCIE EI CAS 2008年第4期528-531,共4页
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
关键词 gold catalyst deposition precipitation CeO2 catalytic oxidation of HCHO rare earths
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Investigation of water adsorption and dissociation on Au_1/CeO_2 single-atom catalysts using density functional theory 认领 引用 被引量：3
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作者 Yan Tang Yang‐Gang Wang +1 位作者 Jin‐Xia Liang Jun Li 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2017年第9期1558-1565,共8页
We examined the water adsorption and dissociation on ceria surfaces as well as ceria‐supported Au single‐atom catalysts using density functional theory calculations.Molecular and dissociative water were observed to ... We examined the water adsorption and dissociation on ceria surfaces as well as ceria‐supported Au single‐atom catalysts using density functional theory calculations.Molecular and dissociative water were observed to coexist on clean CeO2and reduced Au1/CeO2?x surfaces because of the small difference in adsorption energies,whereas the presence of dissociative water was highly favorable on reduced CeO2?x and clean Au1/CeO2surfaces.Positively charged Au single atoms on the ceria surface not only provided activation sites for water adsorption but also facilitated water dissociation by weakening the intramolecular O-H bonds.In contrast,negatively charged Au single atoms were not reactive for water adsorption because of the saturation of Au5d and6s electron shells.This work provides a fundamental understanding of the interaction between water and single‐atom Au catalysts. 展开更多
关键词 Single‐atom catalyst Au single atom Ceria H2O dissociation
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CeO_2-ZrO_2-La_2O_3-Al_2O_3 composite oxide and its supported palladium catalyst for the treatment of exhaust of natural gas engined vehicles 认领 引用 被引量：5
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作者 Xiaoyu Zhang Enyan,Long +5 位作者 Yile Li Jiaxiu Guo Lijuan Zhang Maochu Gong Minghua Wang Yaoqiang Chen 《Journal of Natural Gas Chemistry》 2009年第2期139-144,共6页
Composite supports CeO2-ZrO2-Al2O3（CZA） and CeO2-ZrO2-Al2O3-La2O3（CZALa） were prepared by co-precipitation method. Palladium catalysts were prepared by impregnation and their purification ability for CH4, CO and N... Composite supports CeO2-ZrO2-Al2O3（CZA） and CeO2-ZrO2-Al2O3-La2O3（CZALa） were prepared by co-precipitation method. Palladium catalysts were prepared by impregnation and their purification ability for CH4, CO and NOx in the mixture gas simulated the exhaust from natural gas vehicles （NGVs） operated under stoichiometric condition was investigated. The effect of La2O3 on the physicochemical properties of supports and catalysts was characterized by various techniques. The characterizations with X-ray diffraction （XRD） and Raman spectroscopy revealed that the doping of La2O3 restrained effectively the sintering of crystallite particles, maintained the crystallite particles in nanoscale and stabilized the crystal phase after calcination at 1000 ℃. The results of N2-adsorption, H2-temperatnre-programmed reduction （H2-TPR） and oxygen storage capacity （OSC） measurements indicated that La2O3 improved the textural properties, reducibility and OSC of composite supports. Activity testing results showed that the catalysts exhibit excellent activities for the simultaneous removal of methane, CO and NOx in the simulated exhaust gas. The catalysts supported on CZALa showed remarkable thermal stability and catalytic activity for the three pollutants, especially for NOx. The prepared palladium catalysts have high ability to remove NOx, CH4 and CO, and they can be used as excellent catalysts for the purification of exhaust from NGVs operated under stoichiometric condition. The catalysts reported in this work also have significant potential in industrial application because of their high performance and low cost. 展开更多
关键词 Pd catalysts natural gas vehicles exhaust methane oxidation NOx conversion CeO2-ZrO2-Al2O3 La2O3
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Catalytic Oxidative Properties and Characterization of CuO/CeO_2 Catalysts 认领 引用 被引量：8
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作者 蒋晓原 周仁贤 +2 位作者 袁骏 吕光烈 郑小明 《Journal of Rare Earths》 SCIE EI CAS 2003年第1期55-59,共5页
The oxidative properties and characterization of CuO, CeO 2 and CuO/CeO 2 cata lysts were examined by means of a CO micro-reactor GC system, TPR, XPS and X-r ay diffraction Rietveld methods. The results show that eith... The oxidative properties and characterization of CuO, CeO 2 and CuO/CeO 2 cata lysts were examined by means of a CO micro-reactor GC system, TPR, XPS and X-r ay diffraction Rietveld methods. The results show that either CuO or CeO 2 ac tivity is quite low for CO oxidation. However, when CuO and CeO 2 are mixed, the oxidative activity of the catalyst increases significantly, probably owing to the valency status of copper species (Cu 2+ and Cu+) on the CeO 2 surfa ce, the dispersion and reducibility. XPS surface analysis shows that CuO loading is very important in forming of either Cu 2+ or Cu+. Rietveld analysis s hows that some CuO, which has smaller ion radius than Ce 4+, enters the Ce O 2 lattice after CuO and CeO 2 are mixed. When the CuO loading reaches 5.0%, the size of CuO crystals is a minimum (6.1 nm) and the micro-strain value i s a maximum (2.86×10 -3), resulting in high surface energy and the best ac tivity for CO oxidation. 展开更多
关键词 physical chemistry CuO/CeO 2 catalysts CO micro-reactor GC system rare earths
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Promoting effect of microwave irradiation on CeO2-TiO2 catalyst for selective catalytic reduction of NO by NH3 认领 引用 被引量：20
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作者 Jie Cheng Liyun Song +5 位作者 Rui Wu Shining Li Yanming Sun Hongtai Zhu Wenge Qiu Hong He 《Journal of Rare Earths》 SCIE EI CAS CSCD 2020年第1期59-69,共11页
In this work we prepared several CeO2-TiO2 catalysts for the NH3-SCR reactionusing co-precipitation with assistance of microwave irradiation.The catalytic NH3-SCR activities over CeO2-TiO2 catalysts at low temperature... In this work we prepared several CeO2-TiO2 catalysts for the NH3-SCR reactionusing co-precipitation with assistance of microwave irradiation.The catalytic NH3-SCR activities over CeO2-TiO2 catalysts at low temperatures are largely enhanced by the treatment of microwave irradiation,the operation temperature window is also broadened.For better understanding the promotion mechanism,the catalyst prepared by conventional co-precipitation with and without microwave irradiation treatment was characterized with H2-TPR,NH3-TPD,XPS,XRD and BET.Microwave irradiation treatment accelerates the crystallite rate of CeO2-TiO2 catalysts,and greatly enlarges their surface area by adjusting their microstructures.The resistance to SO2 and H2O is also improved via regulating the hierarchical pore structure by the microwave irradiation.Microwave irradiation treatment can also improve the redox property and increase the acid sites over the catalyst surfaces.The result of in situ DRIFTS suggests that the microwave irradiation treatment generates more Br?nsted acid sites on CeO2-TiO2-2 h catalyst,helpful in SCR reactions.XPS results show that after microwave irradiation on the CeO2-TiO2 catalysts,the surface demonstrates an elevated concentration of chemisorbed oxygen,consequently leading to better oxidation of NO to NO2.Additionally,the molar ratio of Ce3+/Ce4+has been elevated after being treated by microwave irradiation,a vital factor in enhancing the NH3-SCR activities. 展开更多
关键词 SCR catalyst NH3-SCR Low temperature CeO2-TiO2 Microwave irradiation Rare earths
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CeO2分散度对Au/CeO2-SiO2催化剂上甲醛的催化氧化影响 认领 引用 被引量：4
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作者 张娜 罗孟飞 鲁继青 《中国稀土学报》 CAS CSCD 北大核心 2011年第6期674-680,共7页
采用浸渍法在高比表面积的SiO2上负载不同量的CeO2,得到了CeO2不同颗粒尺寸的CeO2-SiO2载体,并用沉积沉淀法制备了CeO2-SiO2负载的纳米金催化剂。通过元素分析、X射线衍射、程序升温还原、N2物理吸附、拉曼光谱和透射电镜等技术对催化... 采用浸渍法在高比表面积的SiO2上负载不同量的CeO2,得到了CeO2不同颗粒尺寸的CeO2-SiO2载体,并用沉积沉淀法制备了CeO2-SiO2负载的纳米金催化剂。通过元素分析、X射线衍射、程序升温还原、N2物理吸附、拉曼光谱和透射电镜等技术对催化剂进行了表征,并考察了催化甲醛氧化活性。结果表明,高分散度、小尺寸的CeO2有利于得到较小尺寸的Au颗粒,并增强了催化剂的还原能力和氧缺位浓度,从而有利于提高催化剂低温甲醛催化氧化活性。 展开更多
关键词 Au/CeO2催化剂 载体分散度 甲醛 催化氧化 稀土
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Influence of preparation methods on the physicochemical properties and catalytic performance of MnO_x-CeO_2 catalysts for NH_3-SCR at low temperature 认领 引用 被引量：59
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作者 Xiaojiang Yao Kaili Ma +4 位作者 Weixin Zou Shenggui He Jibin An Fumo Yang Lin Dong 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2017年第1期146-159,共14页
This work examines the influence of preparation methods on the physicochemical properties and catalytic performance of MnOx‐CeO2 catalysts for selective catalytic reduction of NO by NH3 (NH3‐SCR) at low temperature.... This work examines the influence of preparation methods on the physicochemical properties and catalytic performance of MnOx‐CeO2 catalysts for selective catalytic reduction of NO by NH3 (NH3‐SCR) at low temperature. Five different methods, namely, mechanical mixing, impregnation,hydrothermal treatment, co‐precipitation, and a sol‐gel technique, were used to synthesizeMnOx‐CeO2 catalysts. The catalysts were characterized in detail, and an NH3‐SCR model reaction waschosen to evaluate the catalytic performance. The results showed that the preparation methodsaffected the catalytic performance in the order: hydrothermal treatment > sol‐gel > co‐precipitation> impregnation > mechanical mixing. This order correlated with the surface Ce3+ and Mn4+ content,oxygen vacancies and surface adsorbed oxygen species concentration, and the amount of acidic sitesand acidic strength. This trend is related to redox interactions between MnOx and CeO2. The catalystformed by a hydrothermal treatment exhibited excellent physicochemical properties, optimal catalyticperformance, and good H2O resistance in NH3‐SCR reaction. This was attributed to incorporationof Mnn+ into the CeO2 lattice to form a uniform ceria‐based solid solution (containing Mn‐O‐Cestructures). Strengthening of the electronic interactions between MnOx and CeO2, driven by thehigh‐temperature and high‐pressure conditions during the hydrothermal treatment also improved the catalyst characteristics. Thus, the hydrothermal treatment method is an efficient and environment‐friendly route to synthesizing low‐temperature denitrification (deNOx) catalysts. 展开更多
关键词 MnOx‐CeO2 catalyst Preparation method Nitrogen oxides Low‐temperature NH3‐SCR Electron interaction Surface acidity
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焙烧温度对Au/CeO_2-La_2O_3催化剂水煤气变换性能的影响 认领 引用 被引量：4
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作者 张卿 何振亮 +2 位作者 林性贻 李锦卫 郑起 《中国稀土学报》 CAS 北大核心 2007年第5期556-561,共6页
采用沉积沉淀法制备了Au/CeO2催化剂,通过N2物理吸附、XRD、H2-TPR和HRTEM等手段研究了焙烧温度对催化剂的织构、物相、还原性能以及WGS反应活性的影响。结果表明,焙烧温度对催化剂活性影响显著,低温焙烧有利于金粒子在载体表面的良好分... 采用沉积沉淀法制备了Au/CeO2催化剂,通过N2物理吸附、XRD、H2-TPR和HRTEM等手段研究了焙烧温度对催化剂的织构、物相、还原性能以及WGS反应活性的影响。结果表明,焙烧温度对催化剂活性影响显著,低温焙烧有利于金粒子在载体表面的良好分散,高温焙烧则会使金粒子在载体表面聚集长大。选择适中的焙烧温度不仅可以使表面纳米金粒子获得较好的分散,而且可使Au与载体间具有适宜的相互作用,从而拥有较佳的WGS性能。在本文考察范围内,300℃焙烧4 h制得的样品在各个反应温度点上均表现了最高的WGS活性。 展开更多
关键词 水煤气变换 Au/CeO2-La2O3催化剂 焙烧温度 稀土
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Preparation, Characterization of CuO/CeO_2 and Cu/CeO_2 Catalysts and Their Applications in Low-Temperature CO Oxidation 认领 引用 被引量：9
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作者 郑修成 韩东战 +4 位作者 王淑萍 张守民 王淑荣 黄唯平 吴世华 《Journal of Rare Earths》 SCIE EI CAS 2005年第1期47-51,共5页
CeO2 was synthesized via sol-gel process and used as supporter to prepare CuO/CeO2, Cu/CeO2 catalysts by impregnation method. The catalytic properties and characterization of CeO2, CuO/CeO2 and Cu/CeO2 catalysts were ... CeO2 was synthesized via sol-gel process and used as supporter to prepare CuO/CeO2, Cu/CeO2 catalysts by impregnation method. The catalytic properties and characterization of CeO2, CuO/CeO2 and Cu/CeO2 catalysts were examined by means of a microreactor-GC system, HRTEM, XRD, TPR and XPS techniques. The results show that CuO has not catalytic activity and the activity of CeO2 is quite low for CO oxidation. However, the catalytic activity of CuO/CeO2 and Cu/ CeO2 catalysts increases significantly. Furthermore, the activity of CuO/CeO2 is higher than that of Cu/CeO2 catalysts. 展开更多
关键词 catalytic chemistry CuO/CeO2 catalysts Cu/CeO2 catalysts carbon monoxide oxidation rare earths
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Effects of WOx modification on the activity, adsorption and redox properties of CeO_2 catalyst for NO_x reduction with ammonia 认领 引用 被引量：26
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作者 Ziran Ma Duan Weng +1 位作者 Xiaodong Wu Zhichun Si 《Journal of Environmental Sciences》 SCIE EI CAS CSCD 2012年第7期1305-1316,共12页
A series of WO3/CeO2 （WOx/CeO2） catalysts were synthesized by wet impregnation of ammonium metatungstate on a CeO2 support. The resulting solid acid catalysts were characterized by X-ray diffraction （XRD）, UV-Vis ... A series of WO3/CeO2 （WOx/CeO2） catalysts were synthesized by wet impregnation of ammonium metatungstate on a CeO2 support. The resulting solid acid catalysts were characterized by X-ray diffraction （XRD）, UV-Vis spectroscopy （UV-Vis）, Raman spectroscopy （Raman）, in-situ Fourier transform infrared spectroscopy （in-situ FT-IR） of ammonia adsorption, NH3-TPD, H2 temperature- programmed reduction （H2-TPR）, NH3/NO oxidation and activity measurements for NOx reduction by NH3 （NH3-SCR）. The results show that polytungstate （WOx） species are the main species of tungsten oxide on the surface of ceria. The addition of tungsten oxide enhances the BriSnsted acidity of ceria catalysts remarkably and decreases the amount of surface oxygen on celia, with strong interaction between CeO2 and WOx. As a result, the N2 selectivity of NH3 oxidation and NH3-SCR at high temperatures （〉 300℃） is enhanced. Therefore, a wide working temperature window in which NOx conversion exceeds 80% （NOx conversion 〉 80%） from 200 to 450℃, is achieved over 10 wt.% WOx/CeO2 catalyst. A tentative model of the NH3-SCR reaction route on WOx/CeO2 catalysts is presented. 展开更多
关键词 NOx reduction WOx/CeO2 catalyst redox NH3 adsorption
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Au/CeO2催化剂有氧条件下催化水煤气变换反应的研究 认领 引用 被引量：2
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作者 李凯 王攀 +2 位作者 李振国 崔宸睿 雷利利 《江苏大学学报（自然科学版）》 CAS 北大核心 2020年第6期655-660,共6页
通过沉积沉淀法制备了Au负载量为3%的Au/CeO2催化剂,并利用表征手段结合固定床反应器试验研究了催化剂的理化特性和催化水煤气变换反应(water gas shift reaction,WGSR)的活性.结果表明:Au元素均匀地分散在了载体表面,改善了催化剂的氧... 通过沉积沉淀法制备了Au负载量为3%的Au/CeO2催化剂,并利用表征手段结合固定床反应器试验研究了催化剂的理化特性和催化水煤气变换反应(water gas shift reaction,WGSR)的活性.结果表明:Au元素均匀地分散在了载体表面,改善了催化剂的氧化还原性能和CO吸附性能,进而提高了催化剂的活性,当反应温度为300℃时,WGSR试验中CO转化率提高了56.0%,O2促进了催化剂表面碳酸盐类物质的分解,恢复了催化剂的表面活性位,明显提高了低温下CO的转化率;当反应温度在200,250℃时,CO转化率分别提高了15.0%和17.5%. 展开更多
关键词 Au/CeO2催化剂 CO氧化 低温 氧气 WGSR
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Promotional effect of CO pretreatment on CuO/CeO_2 catalyst for catalytic reduction of NO by CO 认领 引用 被引量：14
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作者 顾贤睿 李昊 +3 位作者 刘礼晨 汤常金 高飞 董林 《Journal of Rare Earths》 SCIE EI CAS CSCD 2014年第2期139-145,共7页
The CuO/CeO2 catalysts were investigated by means of X-ray diffraction （XRD）, laser Raman spectroscopy （LRS）, X-ray photoelectronic spectroscopy （XPS）, temperature-programmed reduction （TPR）, in situ Fourier t... The CuO/CeO2 catalysts were investigated by means of X-ray diffraction （XRD）, laser Raman spectroscopy （LRS）, X-ray photoelectronic spectroscopy （XPS）, temperature-programmed reduction （TPR）, in situ Fourier transform infrared spectroscopy （FTIR） and NO＋CO reaction. The results revealed that the low temperature （〈150℃） catalytic performances were enhanced for CO pretreated samples. During CO pretreatment, the surface Cu＋/Cu0 and oxygen vacancies on ceria surface were present. The low va- lence copper species activated the adsorbed CO and surface oxygen vacancies facilitated the NO dissociation. These effects in turn led to higher activities of CuO/CeO2 for NO reduction. The current study provided helpful understandings of active sites and reaction mechanism in NO＋CO reaction. 展开更多
关键词 CuO/CeO2 catalysts CO pretreatment oxygen vacancies NO reduction rare earths
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Au/CeO_2-TiO_2表面物种在还原和CO氧化过程中的变化 认领 引用 被引量：4
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作者 俞俊 吴贵升 +1 位作者 毛东森 卢冠忠 《化学学报》 SCIE CAS 北大核心 2009年第13期1407-1411,共5页
采用溶胶-凝胶法制备了CeO2-TiO2载体,再用沉积沉淀法制备了Au/CeO2-TiO2催化剂.利用原位漫反射红外(FT-IR),程序升温还原(TPR)、X射线衍射(XRD)、N2吸附-脱附方法考察了催化剂的结构和表面性能.结果表明,CeO2的存在有效抑制TiO2晶粒的... 采用溶胶-凝胶法制备了CeO2-TiO2载体,再用沉积沉淀法制备了Au/CeO2-TiO2催化剂.利用原位漫反射红外(FT-IR),程序升温还原(TPR)、X射线衍射(XRD)、N2吸附-脱附方法考察了催化剂的结构和表面性能.结果表明,CeO2的存在有效抑制TiO2晶粒的长大,增加TiO2的比表面积和晶格应变,从而增强了Au和载体中TiO2的相互作用,使得催化剂表面的氧化能力显著增强.结合原位CO吸附的FT-IR结果表明,不同温度的还原预处理能有效改变催化剂表面氧物种的组成,并对不同氧物种在CO低温氧化过程中的作用进行了分析. 展开更多
关键词 Au催化剂 CO氧化 CeO2-TiO2载体 表面物种
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Effect of CeO2-ZrO2 on Pt/C electrocatalysts for alcohols oxidation 认领 引用 被引量：7
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作者 王青春 刘振朋 +3 位作者 安胜利 王瑞芬 王艳玲 徐拓 《Journal of Rare Earths》 SCIE EI CAS CSCD 2016年第3期276-282,共7页
The electrocatalytic activity and stability of Pt/C catalyst modified by using CeO_2-ZrO_2 mixed oxides for the alcohols electrochemical oxidation as probes were investigated. The catalyst samples were characterized b... The electrocatalytic activity and stability of Pt/C catalyst modified by using CeO_2-ZrO_2 mixed oxides for the alcohols electrochemical oxidation as probes were investigated. The catalyst samples were characterized by X-ray diffraction（XRD） and scanning electron microscopy（SEM）. The electrochemical properties were measured by a three electrode system on electrochemical workstation（IVIUM）. The results showed that the presence of CeO_2-ZrO_2 might be associated with the presence of Pt, which indicated that possibly there was synergistic effect between CeO_2-ZrO_2 and Pt nanoparticles. The electrocatalytic activity and stability of Pt-MO_x/C（M=Ce, Zr） for methanol and ethanol oxidation was better than that of Pt-CeO_2/C, which was attributed to that CeO_2-ZrO_2 composited oxides enhanced oxygen mobility and promoted oxygen storage capacity（OSC）. Furthermore, the best performance was found when the molar ratio of CeO_2 to ZrO_2 was 2：1 for the oxidation of methanol and ethanol. The forward peak current density of Pt-MO_x/C（M=Ce, Zr, Ce：Zr=2：1） towards the methanol electrooxidation was about 3.8 times that of Pt-CeO_2/C. Pt-MO_x/C（M=Ce, Zr） appeared to be a promising and less expensive methanol oxidation anode catalyst. 展开更多
关键词 CeO2-ZrO2 composite oxide catalyst preparation characterization performance rare earths
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碳纳米管改性对Au/CeO_2催化剂乙醇部分氧化制氢的影响 认领 引用 被引量：3
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作者 蔡建信 罗来涛 张荣斌 《化工学报》 EI CSCD 北大核心 2011年第1期92-96,共5页
采用沉积沉淀法制备了一系列碳纳米管改性的Au/CeO2催化剂,以乙醇部分氧化制氢为探针反应,研究了碳纳米管对Au/CeO2催化剂乙醇部分氧化性能的影响,并运用XRD、TPR、BET等方法对催化剂进行了表征。结果表明,碳纳米管的添加提高了Au/CeO2... 采用沉积沉淀法制备了一系列碳纳米管改性的Au/CeO2催化剂,以乙醇部分氧化制氢为探针反应,研究了碳纳米管对Au/CeO2催化剂乙醇部分氧化性能的影响,并运用XRD、TPR、BET等方法对催化剂进行了表征。结果表明,碳纳米管的添加提高了Au/CeO2催化剂的比表面积、孔容和吸氧量,催化剂的氢气选择性先随碳纳米管添加量的增加而大幅增加,碳纳米管的添加量达6%～10%时,氢气选择性达到43%。进一步提高碳纳米管的含量,氢气选择性增加幅度不大。碳纳米管的添加可以有效抑制副产物CO的产生。 展开更多
关键词 碳纳米管 Au/CeO2催化剂 乙醇部分氧化 制氢
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CeO_2@Au核壳结构纳米粒子的合成与性质研究 认领 引用 被引量：6
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作者 杨晓峰 董相廷 +2 位作者 黄磊 王进贤 刘桂霞 《中国稀土学报》 EI CAS 北大核心 2008年第6期683-688,共6页
采用沉淀法制备了球形CeO2纳米粒子,将其作为核粒子溶液,然后向其中滴加四氯合金酸溶液,在CeO2胶体表面利用柠檬酸钠还原[AuCl4]-离子,得到了CeO2@Au核壳结构纳米粒子。TEM分析表明,CeO2纳米粒子分散效果好,粒径为5 nm;CeO2@Au核壳粒子... 采用沉淀法制备了球形CeO2纳米粒子,将其作为核粒子溶液,然后向其中滴加四氯合金酸溶液,在CeO2胶体表面利用柠檬酸钠还原[AuCl4]-离子,得到了CeO2@Au核壳结构纳米粒子。TEM分析表明,CeO2纳米粒子分散效果好,粒径为5 nm;CeO2@Au核壳粒子为球形,无团聚,平均粒径为15 nm。XRD分析表明,CeO2@Au核壳粒子为晶型结构,属于立方晶系,CeO2空间群为O5H-FM3M,Au的空间群为Fm-3m。UV-vis分析发现,CeO2@Au核壳粒子在300和520 nm处呈现出两个比较强的吸收峰,分别对应于CeO2胶体溶液的吸收峰和金粒子的表面等离子共振吸收峰。EDS分析了核壳结构CeO2@Au纳米粒子中存在Ce,O和Au 3种元素。XPS分析表明,Ce3d3/2和Au4f电子结合能与标准结合能相比发生了变化,说明CeO2与Au之间存在着相互作用。 展开更多
关键词 核壳纳米粒子 纳米粒子 CeO2 CeO2@Au Au 稀土
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Mechanistic insight into N_2O formation during NO reduction by NH_3 over Pd/CeO_2 catalyst in the absence of O_2 认领 引用 被引量：10
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作者 Liping Sheng Zhaoxia Ma +6 位作者 Shiyuan Chen Jinze Lou Chengye Li Songda Li Ze Zhang Yong Wang Hangsheng Yang 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2019年第7期1070-1077,共8页
N2O is a major by-product emitted during low-temperature selective catalytic reduction of NO with NH3(NH3-SCR), which causes a series of serious environmental problems. A full understanding of the N2O formation mechan... N2O is a major by-product emitted during low-temperature selective catalytic reduction of NO with NH3(NH3-SCR), which causes a series of serious environmental problems. A full understanding of the N2O formation mechanism is essential to suppress the N2O emission during the low-temperature NH3-SCR, and requires an intensive study of this heterogeneous catalysis process. In this study, we investigated the reaction between NH3 and NO over a Pd/CeO2 catalyst in the absence of O2, using X-ray photoelectron spectroscopy, NH3-temperature-programmed desorption, NO-temperature-programmed desorption, and in-situ Fourier-transform infrared spectroscopy. Our results indicate that the N2O formation mechanism is reaction-temperature-dependent. At temperatures below 250 ℃, the dissociation of HON, which is produced from the reaction between surface H· adatoms and adsorbed NO, is the key process for N2O formation. At temperatures above 250 ℃,the reaction between NO and surface N·, which is produced by NO dissociation, is the only route for N2O formation, and the dissociation of NO is the rate-determining step. Under optimal reaction conditions, a high performance with nearly 100% NO conversion and 100% N2 selectivity could be achieved. These results provide important information to clarify the mechanism of N2O formation and possible suppression of N2 O emission during low-temperature NH3-SCR. 展开更多
关键词 N2O formation NO reduction Pd/CeO2 catalyst in-situ IR spectroscopy Mechanism
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Identification of relevant active sites and a mechanism study for reverse water gas shift reaction over Pt/CeO_2 catalysts 认领 引用 被引量：10
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作者 Xiaodong Chen Xiong Su +5 位作者 Binglian Liang Xiaoli Yang Xinyi Ren Hongmin Duan Yanqiang Huang Tao Zhang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2016年第6期1051-1057,共7页
Reverse water gas shift (RWGS) reaction can serve as a pivotal stage in the CO2 conversion processes, which is vital for the utilization of CO2. In this study, RWGS reaction was performed over Pt/CeO2 catalysts at the... Reverse water gas shift (RWGS) reaction can serve as a pivotal stage in the CO2 conversion processes, which is vital for the utilization of CO2. In this study, RWGS reaction was performed over Pt/CeO2 catalysts at the temperature range of 200-500 degrees C under ambient pressure. Compared with pure CeO2, Pt/CeO2 catalysts exhibited superior RWGS activity at lower reaction temperature. Meanwhile, the calculated TOF and E-a values are approximately the same over these Pt/CeO2 catalysts pretreated under various calcination conditions, indicating that the RWGS reaction is not affected by the morphologies of anchored Pt nanoparticles or the primary crystallinity of CeO2. TPR and XPS results indicated that the incorporation of Pt promoted the reducibility of CeO2 support and remarkably increased the content of Ce 3 + sites on the catalyst surface. Furthermore, the CO TPSR-MS signal under the condition of pure CO2 flow over Pt/CeO 2 catalyst is far lower than that under the condition of adsorbed CO2 with H-2 -assisted flow, revealing that CO2 molecules adsorbed on Ce3+ active sites have difficult in generating CO directly. Meanwhile, the adsorbed CO2 with the assistance of H-2 can form formate species easily over Ce3+ active sites and then decompose into Ce3+-CO species for CO production, which was identified by in-situ FTIR. (C) 2016 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B. V. and Science Press. All rights reserved. 展开更多
关键词 RWGS reaction Pt/CeO2 catalyst Formate intermediate Mechanism
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