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Hydrogen-driven metal-support interaction in Ni-CeO2 catalysts boosting low-temperature CO2 methanation 认领 引用
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作者 Ru Zhao Siyuan Xu +5 位作者 Junliang Xia Mingxue Wang Xiaoyan Han Yu Xie Qiulin Zhang Ping Ning 《Journal of Rare Earths》 SCIE EI CAS CSCD 2026年第7期2097-2105,I0004,共9页
Converting CO2 to CH4 under mild conditions represents a promising strategy for carbon emission reduction and synthetic natural gas production,yet it remains challenging.In this work,we accelerated low-temperatu... Converting CO2 to CH4 under mild conditions represents a promising strategy for carbon emission reduction and synthetic natural gas production,yet it remains challenging.In this work,we accelerated low-temperature CO2 hydrogenation over Ni-CeO2 catalysts by optimizing metal-support interactions through H2-driven reconstruction.The catalyst reduced at 400℃(Ni-CeO2-400R)achieved 84.3%CO2conversion with 100%CH4 selectivity even at a low temperature of 250℃.Various in situ spectroscopic characterizations(X-ray photoelectron spectroscopy(XPS),Raman,and diffused reflectance infrared Fourier transform spectroscopy(DRIFTS))and H2/D2 isotopic exchange experiments reveal that the appropriate interaction in Ni-CeO2 motivates the dispersion of metallic Ni sites and the generation of oxygen vacancies,thereby promoting the activation of H2 and CO2 molecules,respectively.Therefore,CO2 is efficiently adsorbed and converted into reactive intermediates and finally hydrogenated to CH4through carbonyl and formate pathways simultaneously.These findings underscore the critical role of tailored metal-support interactions in designing advanced CO2 hydrogenation catalysts. 展开更多
关键词 Low-temperature CO2methanation Ni/CeO2catalysts H2treatment Metal-support interaction Rare earths
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Size-Dependent Hydrogen Dissociation Capacity in Ni/CeO2 Catalysts for Low-Temperature CO2 Methanation 认领 引用
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作者 Yu Xie Zhiyu Li +6 位作者 Xiaoyan Han Mingxue Wang Ru Zhao Siyuan Xu Qiulin Zhang Ping Ning Jiming Hao 《Rare Metals》 SCIE EI CAS CSCD 2026年第2期718-732,共15页
Converting CO2to CH4 under mild conditions is a promising strategy for solving environmental and energy problems,but also a challenge.In this work,the low-temperature CO2 hydrogenation process over Ni/CeO2 ca... Converting CO2to CH4 under mild conditions is a promising strategy for solving environmental and energy problems,but also a challenge.In this work,the low-temperature CO2 hydrogenation process over Ni/CeO2 catalysts was significantly accelerated by optimizing the H2 dissociation ability of Ni through the size effect,thus A-Ni/CeO2 with an average size of 4.9 nm achieved 83.4%CO2conversion with~100%CH4 selectivity even at 225℃.Systematic H2/D2 isotopic exchange experiments,in situ spectroscopic characterizations,and density functional theory(DFT)calculations reveal that the enhanced H2 activation ability not only promoted the creation of oxygen vacancies and hydroxyl group favorable for CO2 adsorption/activation in the pre-reduction process,but also the simultaneous hydrogenation of reactive intermediates belonging to carbonyl and formate pathway into CH4 in the reaction process.This fundamental understanding of the H2 dissociation effect on CO2 activation and hydrogenation provides critical insights for designing catalysts with considerable low-temperature activity,which significantly reduces energy consumption and operating costs for industrial CO2 conversion. 展开更多
关键词 CO2activation H2dissociation low-temperature CO2methanation Ni/CeO2catalysts size effect
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CO2-assisted two-step pyrolysis fabrication of hierarchical porous Ni/ZrO2catalyst for low-temperature dry reforming of methane 认领 引用
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作者 Xinrong He Bang Xu +4 位作者 Sanli Tang Xiaoguang Liu Qibin Liu Zongguo Wen Maohong Fan 《Journal of Environmental Sciences》 SCIE EI CAS CSCD 2026年第5期163-174,共12页
A new strategy for preparing highly dispersed,richer oxygen vacancies Ni/ZrO2catalysts derived from UiO-66-NH2is reported via pyrolysis-calcination removal of the ligands under N2,CO2,and Air atmospheres f... A new strategy for preparing highly dispersed,richer oxygen vacancies Ni/ZrO2catalysts derived from UiO-66-NH2is reported via pyrolysis-calcination removal of the ligands under N2,CO2,and Air atmospheres followed by loading Ni with 5 wt.%via wet impregnation method.Subsequently,the low-temperature dry reforming of methane(DRM)reaction over the obtained Ni/ZrO2catalysts was preliminarily investigated.The results indicated that the Ni/ZrO2C catalyst,obtained by two-step pyrolysis in CO2,contained smaller Ni particles with a size of only 5-7 nm and possessed a hierarchical porous structure,as well as richer oxygen vacancies and basic active sites compared to the other two catalysts.Its catalytic activity in the DRM reaction presented the highest initial conversion of CH4(35%)and CO2(26%)at 600℃,which was 5%higher than that of the Ni/ZrO2-N and Ni/ZrO2-O catalysts obtained by two-step pyrolysis under an N2atmosphere and one-step pyrolysis under an air atmosphere,respectively.Meanwhile,an in-situ DRIFTS experiment revealed that Ni/ZrO2-C could enhance the adsorption and activation of CO2by promoting the formation of formate as an intermediate of CO hydrogenation and reverse water-gas shift(RWGS)reactions,which in turn facilitates the decomposition of CH4. 展开更多
关键词 Low-temperature dry reforming of methane Pyrolysis UiO-66-NH2 MOF-derived Ni/ZrO2catalysts
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Ni/CaO-ZrO2-Al2O3 catalyst for CO2methanation:Enhanced low-temperature activity and high-temperature sintering resistance 认领 引用
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作者 LI Jia SUI Qingqing +2 位作者 JIANG Yanan BAI Yang LIU Yuan 《燃料化学学报（中英文）》 EI CAS CSCD 北大核心 2026年第6期102-112,共11页
Ni/Al2O3 is regarded as one of the most promising catalysts for industrial application in CO2methanation,but is still plagued by issues of inadequate low-temperature activity and thermal sintering.In response... Ni/Al2O3 is regarded as one of the most promising catalysts for industrial application in CO2methanation,but is still plagued by issues of inadequate low-temperature activity and thermal sintering.In response to these challenges,an Ni/CaO-ZrO2-Al2O3 catalyst with high low-temperature activity and robust high-temperature sintering resistance was prepared by introducing Ca and Zr promoters.Under the reaction conditions of 250 and a space velocity of 30000 mL/(g·h),the CO2conversion and methane space-time yield reached 96%and 257.5 mmol/(g·h),respectively.In addition,the Ca-Zr dual-promoted Ni/CaO-ZrO2-Al2O3 catalyst exhibited a smaller increase in the Ni particle size and less activity loss than the Ca-promoted catalyst in a 200 h aging test at 600.The Ca and Zr promoters can not only improve the Ni dispersion but also enhance the surface basicity,resulting in excellent low-temperature activity.Moreover,the Zr promoter suppresses the transformation of Ca species into CaCO3 through solid-phase reaction under operating conditions,thereby inhibiting Ni sintering and ensuring high-temperature stability.This work provides a new promoter design strategy for the development of high-performance Ni-based catalysts for CO2methanation. 展开更多
关键词 methanation Ni/Al2O3catalyst low-temperature activity sintering resistance
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CaO-stabilized tetragonal ZrO2support for high-performance Ni—Fe alloy catalysts in dry reforming of methane 认领 引用
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作者 Yubin Li Jiawei Wang +5 位作者 Yuxin Kang Nana Chen Ru Yan Li Qiu Sha Li Xiaoliang Yan 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2026年第4期230-242,共13页
Tetragonal ZrO2(t-ZrO2)with abundant oxygen vacancies offers a viable approach to support Ni catalysts for enhanced catalytic performance in dry reforming of methane(DRM).However,the application of t-ZrO2is l... Tetragonal ZrO2(t-ZrO2)with abundant oxygen vacancies offers a viable approach to support Ni catalysts for enhanced catalytic performance in dry reforming of methane(DRM).However,the application of t-ZrO2is limited by its inherent thermal instability.Herein,we evaluated Ni3Fe1alloy supported on m-ZrO2and t-ZrO2stabilized with CaO or Y2O3for DRM.Ni3Fe1/m-ZrO2showed inferior activity,while Ni3Fe1/Y2O3—t-ZrO2retained t-ZrO2structure but exhibited poor stability.In contrast,Ni3Fe1/CaO—tZrO2demonstrated high stability,maintaining CH4 and CO2conversions of 78.0%and 87.2%with H2/CO ratio of 0.95 at 800℃.This is attributed to the CaO dopant,which not only stabilized t-ZrO2phase but also strengthened metal—support interaction at the Ni3Fe1—ZrO2interface,increased oxygen vacancy concentration,and improved surface basicity.Notably,these significantly facilitated CH4 dissociation and CO2activation,establishing an effective balance between carbon formation and gasification,thereby improving the coke resistance of the catalyst. 展开更多
关键词 Ni—Fe alloy Dry reforming of methane Carbon dioxide Tetragonal ZrO2 Catalyst support Catalysis
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Photothermal dry reforming of methane reaction over (Ni/Ce0.8Zr0.2O2)@SiO2 catalysts: The Ni content regulation 认领 引用 被引量：1
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作者 Xiaoyan Tian Yu Shi +1 位作者 Jianming Zhang Fagen Wang 《Green Energy & Environment》 SCIE EI CAS CSCD 2025年第8期1751-1763,共13页
Dry reforming of methane(DRM)converts CH4 and CO2 to syngas.Photothermal DRM,which integrates temperature and light,is a sustainable method for storing solar energy in molecules.However,challenges such as limited l... Dry reforming of methane(DRM)converts CH4 and CO2 to syngas.Photothermal DRM,which integrates temperature and light,is a sustainable method for storing solar energy in molecules.However,challenges such as limited light absorption,low photocarrier separation efficiency,Ni sintering,and carbon deposition hinder DRM stability.Herein,we regulated Ni contents in(Ni/Ce0.8Zr0.2O2)@SiO2 catalysts to enhance the optical characteristics while addressing Ni sintering and carbon deposition issues.The(3Ni/Ce0.8Zr0.2O2)@SiO2 catalyst had insufficient Ni content,while the(9Ni/Ce0.8Zr0.2O2)@SiO2 catalyst showed excessive carbon deposition,leading to lower stability compared to the(6Ni/Ce0.8Zr0.2O2)@SiO2 catalyst,which achieved CH4 and CO2 rates to 231.0 μmol gcat-1s-1 and 294.3 μmol gcat-1s-1 ,respectively,at 973 K,with only 0.2 wt.%carbon deposition and no Ni sintering.This work adjusted Ni contents in(Ni/Ce0.8Zr0.2O2)@SiO2 catalysts to enhance DRM performance,which has implications for improving other reactions. 展开更多
关键词 Photothermal DRM (Ni/Ce0.8Zr0.2O2)@SiO2catalyst Ni regulation Carbon deposition
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Effect of calcination temperature on structure and performance of Ni/TiO_2-SiO_2 catalyst for CO_2 reforming of methane 认领 引用 被引量：6
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作者 Sanbing Zhang Jiankang Wang Xiaolai Wang 《Journal of Natural Gas Chemistry》 2008年第2期179-183,共5页
The influence of calcination temperature on the structure and catalytic behavior of Ni/TiO2-SiO2 catalyst, for CO2 reforming of methane to synthesis gas under atmospheric pressure, was investigated. The results showed... The influence of calcination temperature on the structure and catalytic behavior of Ni/TiO2-SiO2 catalyst, for CO2 reforming of methane to synthesis gas under atmospheric pressure, was investigated. The results showed that the Ni/TiO2-SiO2 catalyst calcined at 700 ℃ had high and stable activity while the catalysts calcined at 550 and 850 ℃ had low and unstable activity. Depending on the calcination temperature, one, two, or three of the following Ni-containing species, NiO, Ni2.44Ti0.72Si0.07O4, and NiTiO3 were identified by combining the temperature programmed reduction （TPR） and X-ray diffraction （XRD） results. Their reducibility decreased in the sequence： NiO〉Ni2.44Ti0.72Si0.07O4〉NiTiO3. It suggests that high and stable activities observed over the Ni/TiO2-SiO2 catalyst calcined at 700 ~C were induced by the formation of Ni2.44Ti0.72Si0.07O4 and smaller NiO species crystallite size. 展开更多
关键词 Ni/TiO2-SiO2 catalyst sol-gel CO2 reforming methane
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Regulating the local environment of Ni single-atom catalysts with heteroatoms for efficient CO2 electroreduction 认领 引用
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作者 Gang Wang Imran Muhammad +2 位作者 Hui-Min Yan Jun Li Yang-Gang Wang 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2025年第7期120-129,共10页
The Ni single-atom catalyst dispersed on nitrogen doped graphene support has attracted much interest due to the high selectivity in electro-catalyzing CO2reduction to CO,yet the chemical inertness of the metal cent... The Ni single-atom catalyst dispersed on nitrogen doped graphene support has attracted much interest due to the high selectivity in electro-catalyzing CO2reduction to CO,yet the chemical inertness of the metal center renders it to exhibit electrochemical activity only under high overpotentials.Herein,we report P-and S-doped Ni single-atom catalysts,i.e.symmetric Ni1/PN4and asymmetric Ni1/SN3C can exhibit high catalytic activity of CO2reduction with stable potential windows.It is revealed that the key intermediate*COOH in CO2electroreduction is stabilized by heteroatom doping,which stems from the upward shift of the axial dz2orbital of the active metal Ni atom.Furthermore,we investigate the potential-dependent free energetics and dynamic properties at the electrochemical interface on the Ni1/SN3C catalyst using ab initio molecular dynamics simulations with a full explicit solvent model.Based on the potential-dependent microkinetic model,we predict that S-atom doped Ni SAC shifts the onset potential of CO2electroreduction from–0.88 to–0.80 V vs.RHE,exhibiting better activity.Overall,this work provides an in-depth understanding of structure-activity relationships and atomic-level electrochemical interfaces of catalytic systems,and offers insights into the rational design of heteroatom-doped catalysts for targeted catalysis. 展开更多
关键词 Ni single-atom catalyst Heteroatom doping CO2electroreduction Ab initio molecular dynamics
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Insights on the effect of Si-Al interaction on Ni/Al2O3/SiC monolithic catalysts for CO2 methanation 认领 引用
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作者 Xiangli Liu Fei Gao +3 位作者 Jingyang Huang Yiqing Zeng Zhaoxiang Zhong Weihong Xing 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2025年第11期171-181,共11页
Monolithic catalysts have been widely investigated for CO2 methanation due to their fast mass and heat transfer rate,but the effect of the interaction between the catalyst layer and the monolithic support has been ... Monolithic catalysts have been widely investigated for CO2 methanation due to their fast mass and heat transfer rate,but the effect of the interaction between the catalyst layer and the monolithic support has been little studied.In this work,Ni/Al2O3/SiC monolithic catalysts,Ni/Al2O3 powder catalysts and Ni/Al2O3/SiC-M catalysts were prepared to explore the effect of Si-Al interaction between the catalyst layer and SiC ceramic for CO2 methanation performance.Ni/Al2O3/SiC exhibited a CO2 conversion of 53% and a CH4 specific reaction rate of 0.05 m mol·g-1·s-1 under conditions of 0.1 M Pa,4 00℃,and a WHSV of 60000 ml·g-1·h-1.The CO2 conversion raised by 0.15-fold and the CH4 specific reaction rate raised by 0.25-fold compared to Ni/Al2O3 with the same catalyst content.SEM,XRD,Raman,and other characterization results revealed that the formation of Si-Al interaction between the catalyst layer and SiC ceramic could weaken the interaction between Ni and Al2O3,thereby improving the catalytic activity of Ni/Al2O3/SiC catalyst.However,the Si-Al interaction was further strengthened during the hightemperature reaction process,which significantly weakened the interaction between Ni and Al2O3,thereby leading to a decline in the catalytic performance of Ni/Al2O3/SiC catalyst during an 80-h stability test.This study provides valuable insights for future research and development of monolithic catalysts. 展开更多
关键词 Carbon dioxide Hydrogenation Monolith Ni/Al2O3/SiC monolithic catalyst Si-Al interaction
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临氢热解制备高分散Ni/SiO2及萘加氢性能 认领 引用
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作者 梁正 罗雷 +2 位作者 王小曼 苏秋成 仇松柏 《中山大学学报（自然科学版）（中英文）》 CAS CSCD 北大核心 2026年第2期124-135,共12页
萘作为煤焦油中含量最为丰富的多环芳烃,不仅是一种环境污染物,也是一种高附加值的化工原料。通过催化加氢,萘可转化为具有更高价值的四氢萘和十氢萘。在各类加氢催化剂中,负载型镍基材料因其成本优势,被视为潜在的非贵金属替代方案。... 萘作为煤焦油中含量最为丰富的多环芳烃,不仅是一种环境污染物,也是一种高附加值的化工原料。通过催化加氢,萘可转化为具有更高价值的四氢萘和十氢萘。在各类加氢催化剂中,负载型镍基材料因其成本优势,被视为潜在的非贵金属替代方案。本研究采用柠檬酸(CA)辅助的溶胶凝胶法,结合临氢热解策略,成功制备了高分散Ni/SiO2催化剂。通过系统表征与催化性能测试,重点探究了柠檬酸用量、热解气氛及临氢热解温度对催化剂物化性质与萘加氢性能的调控规律。结果表明,在优化的柠檬酸配比与H2气氛下热解所得的w=20%Ni/SiO2-CA(H2)催化剂,表现出优于无CA对照组及其他热解工艺催化剂的加氢活性。在相同低温反应条件下,其活性显著高于商业Ru/C催化剂。本研究为开发高效非贵金属加氢催化剂提供了新思路与实验依据。 展开更多
关键词 高分散Ni/SiO2催化剂 溶液凝胶法 临氢热解 萘加氢反应
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Selective Hydrogenation of Butyne-1,4-diol to Butane-1,4-diol over Ni/Al_2O_3-SiO_2 Catalysts 认领 引用 被引量：2
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作者 Fang Jie Zhuang Changjian +2 位作者 Meng Jipeng Cheng Lang Lu Jiangyin 《China Petroleum Processing & Petrochemical Technology》 CAS 2018年第4期20-28,共9页
Ni/Al_2O_3-SiO_2 catalysts were synthesized via one-step method employing SiO_2 as an additive for the selective hydrogenation of butyne-1,4-diol(B_3D) to butane-1,4-diol(B1D). The prepared catalysts were evaluated by... Ni/Al_2O_3-SiO_2 catalysts were synthesized via one-step method employing SiO_2 as an additive for the selective hydrogenation of butyne-1,4-diol(B_3D) to butane-1,4-diol(B1D). The prepared catalysts were evaluated by a series of characterization techniques including BET, XRD, SEM, EDX-mapping, TEM, H_2-TPR, XPS, NH_3-TPD and Py-FTIR. Compared to Ni/Al_2O_3 catalyst, the SiO_2-doped samples exhibited better B_3D conversion. SiO_2 could help to form a strong interaction between NiO with the support, which inhibited Ni agglomeration at high temperature, improved the Ni dispersion, and enhanced the hydrogenation activity. B_1D selectivity was mainly influenced by the quantity of Lewis acid sites in addition to the Ni dispersion. The catalyst with a silica loading of 6.4% demonstrated an excellent selectivity of 75.18%(by 13% higher than the contrastive Ni/Al_2O_3 catalyst), which was attributed to the larger amount of Lewis acid sites and the moderate interaction between NiO with the support, which could facilitate the nickel dispersion on a preferable surface area of 176.3 m^2/g of support. 展开更多
关键词 Ni/Al2O3-SiO2 catalysts butyne-1,4-diol butane-1,4-diol hydrogenation
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Catalytic decomposition of CH_4 over Ni-Al_2O_3-SiO_2 catalysts:Influence of pretreatment conditions for the production of H_2 认领 引用 被引量：2
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作者 Jangam Ashok Gangadhara Raju +2 位作者 Padigapati Shiva Reddy Machiraju Subrahmanyam Akula Venugopal 《Journal of Natural Gas Chemistry》 2008年第2期113-119,共7页
This article reports the production of COx free hydrogen and carbon nanofibers by the catalytic decomposition of methane over Ni-Al2O3-SiO2 catalysts. The influence of reaction temperature, pretreatment temperature, a... This article reports the production of COx free hydrogen and carbon nanofibers by the catalytic decomposition of methane over Ni-Al2O3-SiO2 catalysts. The influence of reaction temperature, pretreatment temperature, and effect of reductive pretreatment on the decomposition of methane activity is investigated. The physico-chemical characteristics of fresh and deactivated samples were characterized using BET-SA, XRD, TPR, SEM/TEM, CHNS analyses and correlated with the methane decomposition results obtained. The Ni-Al-Si （4 ： 0.5 ： 1.5） catalyst reduced with hydrazine hydrate produced better H2 yields of ca. 1815 mol H2/mol Ni than the catalyst reduced with 5% H2/N2. 展开更多
关键词 in situ reduction Ni-Al2O3-SiO2 catalyst methane decomposition hydrogen production carbon nanofibers
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CeO2修饰NiCuMgAl混合金属催化剂及催化甲烷干重整研究 认领 引用
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作者 吴以星 焦卫红 +4 位作者 李彪 毕晨瑶 王艳 张静 刘一鸣 《分子催化（中英文）》 CAS CSCD 北大核心 2026年第3期305-320,I0002,共16页
甲烷干重整反应可将两种温室气体同时转化为合成气,是一种兼具环保效益与资源化利用价值的重要反应,但是该反应仍面临能耗高、催化剂因积炭和烧结易失活等关键挑战.本研究采用尿素水热法制备NiCuMgAl水滑石前驱体,并通过浸渍法引入不同... 甲烷干重整反应可将两种温室气体同时转化为合成气,是一种兼具环保效益与资源化利用价值的重要反应,但是该反应仍面临能耗高、催化剂因积炭和烧结易失活等关键挑战.本研究采用尿素水热法制备NiCuMgAl水滑石前驱体,并通过浸渍法引入不同浓度的硝酸铈溶液,经煅烧还原后得到一系列CeO2负载量分别为5%、10%、15%、20%的NiCuMgAl催化剂,系统考察了CeO2含量对催化剂结构、表面性质及甲烷干重整性能的影响.结合X射线衍射、氮气物理吸附-脱附、扫描电镜、透射电镜、X射线光电子能谱、二氧化碳与氨气程序升温脱附、傅立叶红外光谱和热重对催化剂进行表征.结果表明,Ni-Cu合金的形成有效抑制了积炭生成,CeO2的引入则产生了丰富的氧空位.其中NiCuMgAl-15%Ce催化剂具有最高的氧空位浓度(33.80%),同时表现出最强的中强碱强度(250.4℃)和中强酸强度(240.7℃),形成了理想的酸碱协同效应.该催化剂在600℃、质量空速36000 mL·g-1·h-1条件下,CH4转化率达36.2%,CO2转化率达53.1%,稳定运行32 h,积炭量仅6.2%,显著优于未改性及CeO2含量过高或过低的催化剂. 展开更多
关键词 甲烷干重整反应 Ni基催化剂 合金 CeO2
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MgO、MnO2复合助剂改性Ni基催化剂CO2甲烷化催化性能 认领 引用
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作者 张晓煜 张春磊 +3 位作者 徐则林 马吉亮 许芸 周凯 《低碳化学与化工》 CAS 北大核心 2026年第7期66-73,94,共8页
面对全球气候变化与能源转型的迫切需求,CO2甲烷化工艺能够将富余的电力与CO2转化为易于储存和运输的CH4,有利于构建未来低碳能源体系。然而,现有的Ni基催化剂存在活性组分分散性有限、催化活性不足等问题。采用分步浸渍-焙烧... 面对全球气候变化与能源转型的迫切需求,CO2甲烷化工艺能够将富余的电力与CO2转化为易于储存和运输的CH4,有利于构建未来低碳能源体系。然而,现有的Ni基催化剂存在活性组分分散性有限、催化活性不足等问题。采用分步浸渍-焙烧策略,通过引入MgO与MnO2作为复合助剂,对Ni基催化剂进行了协同改性,制备了一系列不同助剂种类与含量的催化剂。通过XRD、N2吸/脱附和CO2-TPD等方法对催化剂的结构和表面性质进行了表征,并通过固定床反应系统评价了其CO2甲烷化催化性能。结果表明,340℃时,在MgO与MnO2协同改性的5Mg2MnNiAl催化剂作用下,CO2转化率达92.12%,CH4选择性达99.02%。表征分析显示,MgO的引入丰富了催化剂的中强碱性位点,促进了CO2吸附与活化;MnO2则有效细化并均匀分散了Ni颗粒,增强了金属-载体相互作用。本研究将为CO2甲烷化催化剂制备及其工业化应用提供参考。 展开更多
关键词 CO2甲烷化 Ni基催化剂 MgO MnO2 金属-载体相互作用
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CaH2-promoted activity of Ni-carbonate interface for CO2 methanation 认领 引用
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作者 Jin-Peng Wang Guo-Cui Mao +2 位作者 Hui-Lin Jiang Bao-Xia Dong Yun-Lei Teng 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2025年第1期522-532,共11页
Transition metal-carbonate interfaces often act as active sites in heterogeneous catalytic reactions.The interface between transition metal and metal carbonate exhibits a dynamic equilibrium during the CO2hydrogena... Transition metal-carbonate interfaces often act as active sites in heterogeneous catalytic reactions.The interface between transition metal and metal carbonate exhibits a dynamic equilibrium during the CO2hydrogenation reaction,involving surface carbonate hydrogenation and CO2chemisorption.Nonetheless,there have been few reports on engineering the activity of the interface between transition metal and alkaline earth metal carbonate for catalytic CO2conversion.This work demonstrated that the incorporation of CaH2in Ni/CaCO3enhances the CO2methanation activity of the catalysts.The CO2conversion for Ni/CaH2-CaCO3reached 68.5%at 400°C,which was much higher than that of the Ni/CaCO3(31.6%) and Ni/CaH2-CaO (42.4%) catalysts.Furthermore,the Ni/CaH2-CaCO3catalysts remained stable during the stability test for 24 h at 400°C and 8 bar.Our research revealed that CaH2played a crucial role in promoting the activity of the Ni-carbonate interface for CO2methanation.CaH2could modify the electronic structure of Ni and tune the structural properties of CaCO3to generate medium basic sites (OH groups),which are favorable for the activation of H2and CO2.In-situ Fourier transform infrared spectroscopy (FTIR) analysis combined with density functional theory calculations demonstrated that CO2activation occurs at the hydroxyl group (OH) on the CaH2-modified Ni-carbonate surface,leading to the formation of CO3H*species.Furthermore,our study has confirmed that CO2methanation over the Ni/CaH2-CaCO3catalysts proceeds via the formate pathway. 展开更多
关键词 CO2methanation Metal hydride Ni catalysts Carbonate Metal-carbonate interface
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Comparative study of fluidized-bed and fixed-bed reactor for syngas methanation over Ni-W/TiO_2-SiO_2 catalyst 认领 引用 被引量：9
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作者 Bo Liu Shengfu Ji 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2013年第5期740-746,共7页
In this work,syngas methanation over Ni-W/TiO2-SiO2catalyst was studied in a fluidized-bed reactor(FBR)and its performance was compared with a fixed-bed reactor(FIXBR).The effects of main operating variables including... In this work,syngas methanation over Ni-W/TiO2-SiO2catalyst was studied in a fluidized-bed reactor(FBR)and its performance was compared with a fixed-bed reactor(FIXBR).The effects of main operating variables including feedstock gases space velocity,coke content,bed temperature and sulfur-tolerant stability of 100 h life were investigated.The structure of the catalysts was characterized by XRD,N2adsorptiondesorption and TEM.It is found that under same space velocity from 5000 h 1to 25000 h 1FBR gave a higher CH4yield,lower coke content,and lower bed temperature than those obtained in FIXBR.Ni-W/TiO2-SiO2catalyst possessed excellent sulfur-tolerant stability on the feedstock gases less than 500 ppm H2S in FBR.The carbon deposits formed on the spent catalyst were in the form of carbon fibers in FBR,while in the form of dense accumulation distribution appearance in FIXBR. 展开更多
关键词 syngas methanation Ni-W/TiO2-SiO2catalyst fluidized bed fixed bed
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乙醇溶剂体积对Ni-Fe/γ-Al2O3催化剂微波热解高密度聚乙烯制氢性能的影响 认领 引用
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作者 魏家荣 谢翔 +5 位作者 周志彬 雷丁懿 李嘉墀 卢林博 侯丽敏 张智羽 《塑料工业》 CAS CSCD 北大核心 2026年第6期159-166,共8页
微波热解因反应速率快、能效高,被认为是塑料废弃物资源化制氢的重要途径,其中催化剂制备工艺对制氢性能具有关键影响。以Ni-Fe/γ-Al2O3;为研究对象,系统考察乙醇体积(0、25、50、75mL)对催化剂结构及其在高密度聚乙烯(HDPE)微... 微波热解因反应速率快、能效高,被认为是塑料废弃物资源化制氢的重要途径,其中催化剂制备工艺对制氢性能具有关键影响。以Ni-Fe/γ-Al2O3;为研究对象,系统考察乙醇体积(0、25、50、75mL)对催化剂结构及其在高密度聚乙烯(HDPE)微波热解制氢过程中的性能影响。结果表明,不同体积的乙醇可调控活性组分在γ-Al2O3;载体上的分散状态及物相结构,显著影响催化剂制氢性能。当乙醇体积为25mL时,Ni、Fe活性组分分散均匀,形成稳定的FeAl2O3和NiFe2O4复合活性结构,HDPE热解的氢气产量、氢气效率及氢气体积分数分别达到49.7mmol/g、69.6%和82.7%。乙醇用量不足或过量均会导致活性组分分布不均或团聚脱落,从而削弱制氢性能。该研究表明,合理调控乙醇体积是优化Ni-Fe/γ-Al2O3,催化剂制备工艺、提升微波热解塑料制氢效率的有效途径。 展开更多
关键词 Ni-Fe/γ-Al2O3催化剂 乙醇溶剂 微波热解 高密度聚乙烯 制氢性能
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Novel promoting effects of cerium on the activities of NO_x reduction by NH_3 over TiO_2-SiO_2-WO_3 monolith catalysts 认领 引用 被引量：15
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作者 房志涛 林涛 +3 位作者 徐海迪 吴干学 孙萌萌 陈耀强 《Journal of Rare Earths》 SCIE EI CAS CSCD 2014年第10期952-959,共8页
A series of catalysts were prepared by doping different loadings of CeO2 over TiO2-SiO2-WO3 and used for the selective catalytic reduction of NOx by NH3. The experimental results showed that the selective catalytic re... A series of catalysts were prepared by doping different loadings of CeO2 over TiO2-SiO2-WO3 and used for the selective catalytic reduction of NOx by NH3. The experimental results showed that the selective catalytic reduction（SCR） performance and SO2-resistant ability of TiO2-SiO2-WO3 were greatly enhanced by the introduction of cerium. The catalyst containing 10% CeO2 showed the highest NO conversion in a wide temperature range and good N2 selectivity with broad operation temperature window at the gas hourly space velocity（GHSV） of 30000 h–1, which was a very promising catalyst for NOx abatement from diesel engine exhaust. The catalysts were characterized by X-ray diffraction（XRD）, scanning electron microscopy with energy dispersive X-ray spectroscopy（SEM-EDS）, N2 adsorption-desorption（BET） and X-ray photoelectron spectroscopy（XPS）. The characterization results showed that the bigger pore radius, higher surface atomic concentration and dispersion of Ce and the abundant adsorbed oxygen on the surface of catalyst contributed to the best NH3-SCR performance of CeO2/TiO2-SiO2-WO3 catalyst containing 10% CeO2. 展开更多
关键词 NH3-SCR NO cerium CeO2/TiO2-SiO2-WO3 monolith catalyst rare earths
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The Effect of Titania Structure on Ni/TiO_2 Catalysts for p-Nitrophenol Hydrogenation 认领 引用 被引量：12
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作者 陈日志 杜艳 +1 位作者 邢卫红 徐南平 《Chinese Journal of Chemical Engineering》 SCIE EI CAS 2006年第5期665-669,共5页
The catalytic hydrogenation of p-nitrophenol to p-aminophenol was investigated over Ni/TiO2 catalysts prepared by a liquid-phase chemical reduction method. The catalysts were characterized by inductively coupled plasm... The catalytic hydrogenation of p-nitrophenol to p-aminophenol was investigated over Ni/TiO2 catalysts prepared by a liquid-phase chemical reduction method. The catalysts were characterized by inductively coupled plasma (ICP), X-ray powder diffraction (XRD), transmission electron microscopy (TEM), X-ray photoelectron spectra (XPS) and temperature-programmed reduction (TPR). Results show that the titania structure has favorable influence on physio-chemical and catalytic properties of Ni/TiO2 catalysts. Compared to commercial Raney nickel, the catalytic activity of Ni/TiO2 catalyst is much superior, irrespective of the titania structure. The catalytic activity of anatase titania supported nickel catalyst Ni/TiO2(A) is higher than that of rutile titania supported nickel catalyst Ni/TiO2(R), possibly because the reduction of nickel oxide to metallic nickel for Ni/TiO2(A) is easier than that for Ni/TiO2(R) at similar reaction conditions. 展开更多
关键词 p-nitrophenol catalytic hydrogenation p-aminophenol Ni/TiO2 catalyst
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Improving the denitration performance and K-poisoning resistance of the V_2O_5-WO_3/TiO_2 catalyst by Ce4+ and Zr4+ co-doping 认领 引用 被引量：21
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作者 Jun Cao Xiaojiang Yao +4 位作者 Fumo Yang Li Chen Min Fu Changjin Tang Lin Dong 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2019年第1期95-104,共10页
A series of V2O5‐WO3/TiO2‐ZrO2,V2O5‐WO3/TiO2‐CeO2,and V2O5‐WO3/TiO2‐CeO2‐ZrO2 catalysts were synthesized to improve the selective catalytic reduction(SCR)performance and the K‐poisoning resistance of a V2O5‐W... A series of V2O5‐WO3/TiO2‐ZrO2,V2O5‐WO3/TiO2‐CeO2,and V2O5‐WO3/TiO2‐CeO2‐ZrO2 catalysts were synthesized to improve the selective catalytic reduction(SCR)performance and the K‐poisoning resistance of a V2O5‐WO3/TiO2 catalyst.The physicochemical properties were investigated by using XRD,BET,NH3‐TPD,H2‐TPR,and XPS,and the catalytic performance and K‐poisoning resistance were evaluated via a NH3‐SCR model reaction.Ce^4+and Zr^4+co‐doping were found to enhance the conversion of NOx,and exhibit the best K‐poisoning resistance owing to the largest BET‐specific surface area,pore volume,and total acid site concentration,as well as the minimal effects on the surface acidity and redox ability from K poisoning.The V2O5‐WO3/TiO2‐CeO2‐ZrO2 catalyst also presents outstanding H2O+SO2 tolerance.Finally,the in situ DRIFTS reveals that the NH3‐SCR reaction over the V2O5‐WO3/TiO2‐CeO2‐ZrO2 catalyst follows an L‐H mechanism,and that K poisoning does not change the reaction mechanism. 展开更多
关键词 V2O5‐WO3/TiO2‐CeO2‐ZrO2 catalyst Co‐doping K‐poisoning NH3‐SCR Reaction mechanism
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