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Insights into the size effect of ZnCr_(2)O_(4)spinel oxide in composite catalysts for conversion of syngas to aromatics
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作者 Yi Fu Youming Ni +5 位作者 Wenhao Cui Xudong Fang Zhiyang Chen Zhaopeng Liu wenliang zhu Zhongmin Liu 《Green Energy & Environment》 SCIE EI CSCD 2023年第2期530-537,共8页
Direct conversion of syngas to aromatics(STA)over oxide-zeolite composite catalysts is promising as an alternative method for aromatics production.However,the structural effect of the oxide component in composite cata... Direct conversion of syngas to aromatics(STA)over oxide-zeolite composite catalysts is promising as an alternative method for aromatics production.However,the structural effect of the oxide component in composite catalysts is still ambiguous.Herein,we investigate the size effect by selecting ZnCr_(2)O_(4)spinel,as a probe oxide,mixing with H-ZSM-5 zeolite as a composite catalyst for STA reaction.The CO conversion,aromatics selectivity and space-time yield(STY)of aromatics are all significantly improved with the crystal size of ZnCr_(2)O_(4)oxide decreases,which can mainly attribute to the higher oxygen vacancy concentration and thus the rapid generation of more C1oxygenated intermediate species.Based on the understanding of the size-performance relationship,ZnCr_(2)O_(4)-400 with a smaller size mixing with H-ZSM-5 can achieve32.6%CO conversion with 76%aromatics selectivity.The STY of aromatics reaches as high as 4.79 mmol g_(cat)^(-1)h^(-1),which outperforms the previously reported some typical catalysts.This study elucidates the importance of regulating the size of oxide to design more efficient oxidezeolite composite catalysts for conversion of syngas to value-added chemicals. 展开更多
关键词 Size effect Syngas conversion AROMATICS ZnCr_(2)O_(4)oxide H-ZSM-5 zeolite
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Electronic Structure of the Weak Topological Insulator Candidate Zintl Ba_(3)Cd_(2)Sb_(4)
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作者 黄杰瑞 张坦 +9 位作者 徐升 饶志成 李佳俊 刘俊德 高顺业 黄耀波 朱文亮 夏天龙 翁红明 钱天 《Chinese Physics Letters》 SCIE EI CAS CSCD 2023年第4期44-49,共6页
One of the greatest triumph of condensed matter physics in the past ten years is the classification of materials by the principle of topology.The existence of topological protected dissipationless surface state makes ... One of the greatest triumph of condensed matter physics in the past ten years is the classification of materials by the principle of topology.The existence of topological protected dissipationless surface state makes topological insulators great potential for applications and hotly studied.However,compared with the prosperity of strong topological insulators,theoretical predicted candidate materials and experimental confirmation of weak topological insulators(WTIs) are both extremely rare.By combining systematic first-principles calculation and angle-resolved photoemission spectroscopy measurements,we have studied the electronic structure of the dark surface of the WTI candidate Zintl Ba_(3)Cd_(2)Sb_(4)and another related material Ba_(3)Cd_(2)As_(4).The existence of two Dirac surface states on specific side surfaces predicted by theoretical calculations and the observed two band inversions in the Brillouin zone give strong evidence to prove that the Ba_(3)Cd_(2)Sb_(4)is a WTI.The spectroscopic characterization of this Zintl Ba_(3)Cd_(2)N_(4)(N = As and Sb) family materials will facilitate applications of their novel topological properties. 展开更多
关键词 properties TOPOLOGICAL RARE
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用于人工肌肉纤维丝的“三明治”复合结构熔融机理仿真
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作者 韩亚丽 金壮壮 +3 位作者 赵天 孙翰 朱文亮 史传棋 《高分子材料科学与工程》 EI CAS CSCD 北大核心 2022年第1期97-104,共8页
研究了构成“三明治”结构的聚甲基丙烯酸甲酯(PMMA)/聚乙烯(PE)/环烯烃类共聚物弹性体(COCe)3种材料在不同温度场的熔融机理和成型过程,为后续人工肌肉纤维丝的制作提供数据参考。建立了基于标准κ-ε湍流模型的分段加热有限元仿真模型... 研究了构成“三明治”结构的聚甲基丙烯酸甲酯(PMMA)/聚乙烯(PE)/环烯烃类共聚物弹性体(COCe)3种材料在不同温度场的熔融机理和成型过程,为后续人工肌肉纤维丝的制作提供数据参考。建立了基于标准κ-ε湍流模型的分段加热有限元仿真模型,通过设置不同参数对比研究进料速度、单元划分方式和边界条件设置对仿真结果的影响,实现高分子材料加热熔融凝固过程的仿真模拟。仿真结果表明,通过面映射和局部加密处理的方式划分网格得到的计算结果精度较高;控制进料速度约1mm/s时,材料能够得到充分加热,密度达到稳定,有利于材料的挤出成型。 展开更多
关键词 人工肌肉纤维丝 标准κ-ε湍流模型 熔融机理 进料速度
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HZSM-35分子筛酸性质对甲缩醛和乙酸甲酯羟醛缩合反应的影响(英文) 被引量:4
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作者 马占玲 马现刚 +4 位作者 倪友明 刘红超 朱文良 郭新闻 刘中民 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2018年第11期1762-1769,共8页
丙烯酸及其酯是重要的化工原料,广泛应用于涂料、粘结剂、纤维等领域,目前工业上常采用丙烯两段氧化法进行制备,但该法以石油基原料丙烯为源头,采用V/Mo/Bi等金属催化剂,不符合可持续发展理念,且存在环境污染及氧气下产物易过度氧化等问... 丙烯酸及其酯是重要的化工原料,广泛应用于涂料、粘结剂、纤维等领域,目前工业上常采用丙烯两段氧化法进行制备,但该法以石油基原料丙烯为源头,采用V/Mo/Bi等金属催化剂,不符合可持续发展理念,且存在环境污染及氧气下产物易过度氧化等问题.如何高效、安全、大规模工业化制备丙烯酸及其酯是研究者追求的目标.以乙酸甲酯(Mac)和甲醛为原料,通过羟醛缩合一步制备丙烯酸及其酯是一条完全不同于丙烯氧化法的合成路径,原料均可由煤基甲醇得到,符合我国'富煤、贫油、少气'基本能源结构,且该方法碳原子利用率为100%,副产物仅为水,属于绿色环保合成路径.本文以甲缩醛(DMM)为甲醛源,创新性地采用固体硅铝分子筛为酸性催化剂,催化DMM和MAc发生羟醛缩合反应来制备丙烯酸.硅铝分子筛具有较高的活性,可高效地催化羟醛缩合反应,且具有很好的再生性能,即使催化剂寿命较短,也可采用流化床或移动床等反应器进行工业化,因此具有良好的工业化前景.硅铝分子筛中常含有Brnsted酸和Lewis酸,为试图说明羟醛缩合反应的真正活性位点,我们以羟醛缩合反应性能最佳的HZSM-35分子筛为研究目标.首先,利用红外研究HZSM-35分子筛的酸性质.发现分子筛中桥羟基提供Brnsted酸,外骨架铝物种提供Lewis酸.通过对桥羟基红外峰一阶求导,发现其对称性较差,表明Brnsted酸在HZSM-35分子筛孔道中分布不均匀.利用红外分峰手段,得知约51%的Brnsted酸分布于八元环和六元环交叉所形成的笼(cage)中,约23%分布于十元环孔道,26%分布于八元环孔道中.同时,利用吡啶在分子筛HZSM-35不同温度下的吸附情况验证了这一分峰结果.其次,利用钠离子交换方法制备不同Brnsted酸浓度的ZSM-35分子筛,经吡啶红外表征得知,Brnsted酸浓度随钠离子交换程度增加而逐渐降低,而Lewis酸浓度并未改变;在羟醛缩合反应性能中,丙烯酸及丙烯酸甲酯选择性和收率均随Brnsted酸浓度增加而逐渐升高,考虑到Lewis酸浓度并未变化,可知Brnsted酸是羟醛缩合反应性能的活性位点,其浓度增加有利于羟醛缩合反应性能的提高.同时,对比不同ZSM-35分子筛失活现象,高Brnsted酸浓度时分子筛重积炭量最高,这可能是由于Brnsted催化不饱和产物关环生成芳烃物种或(和) 展开更多
关键词 羟醛缩合反应 乙酸甲酯 HZSM-35分子筛 Bronsted位 丙烯酸
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Cs/ZSM-35分子筛催化甲缩醛和乙酸甲酯发生一步法羟醛缩合反应(英文) 被引量:2
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作者 马占玲 马现刚 +3 位作者 刘红超 朱文良 郭新闻 刘中民 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2018年第6期1129-1137,共9页
丙烯酸及其酯是重要的化工原料,广泛应用于涂料、粘结剂、纤维等领域,目前工业上常采用丙烯两段氧化法进行制备.然而该方法以石油基原料丙烯为源头,采用V/Mo/Bi等金属催化剂,不符合可持续发展理念,且存在环境污染及氧气下产物易过度氧... 丙烯酸及其酯是重要的化工原料,广泛应用于涂料、粘结剂、纤维等领域,目前工业上常采用丙烯两段氧化法进行制备.然而该方法以石油基原料丙烯为源头,采用V/Mo/Bi等金属催化剂,不符合可持续发展理念,且存在环境污染及氧气下产物易过度氧化等问题.因此,如何高效、安全、大规模工业化制备丙烯酸及其酯是研究者追求的目标.以乙酸甲酯(MAc)和甲醛为原料,通过羟醛缩合一步制备丙烯酸及其酯是一条完全不同于丙烯氧化法的合成路径,原料均可由煤基甲醇得到,符合我国"富煤、贫油、少气"的基本能源结构,且该方法碳原子利用率为100%,副产物仅为水,属于绿色环保合成路径.羟醛缩合是典型的碳链增长反应,可在酸性催化剂、碱性催化剂、以及酸碱双功能催化剂存在下发生.碱性催化剂一般为负载型碱金属氧化物,例如以SiO_2为载体的负载型Na,K,Cs氧化物催化剂等,但都存在活性组分流失的问题,进而导致催化剂的失活,难以实现工业化.酸碱双功能催化剂是目前研究的热点,由于具有酸催化剂的高选择性和碱催化剂的高活性,其反应性能要远优于单一酸性催化剂和单一碱性催化剂,广大研究者对此进行了深入广泛的研究,目前基本处于实验室阶段.相对而言,目前酸性催化剂上通过羟醛缩合反应制备丙烯酸及其酯的研究工作较少,特别是以固体酸为催化剂进行乙酸甲酯和甲醛气固相反应研究非常少见.我们以甲缩醛为甲醛源,创新性地采用固体硅铝分子筛为酸性催化剂,催化甲缩醛(DMM)和MAc发生羟醛缩合反应来制备丙烯酸.硅铝分子筛具有较高的活性,可高效地催化羟醛缩合反应,且由于分子筛催化剂具有很好的再生性能,即使催化剂寿命较短,也可采用流化床或移动床等反应器进行工业化,因此存在良好的工业化前景.为了进一步深入研究酸性位和碱性位各自对DMM和MAc羟醛缩合反应的影响,本文以HZSM-35分子筛为载体,采用浸渍法制备不同碱金属铯氧化物含量的催化剂,利用氮气吸附/脱附方法和化学程序升温(NH_3-TPD)方法对其孔结构和酸性质进行表征,并进一步考察催化剂的性能.结果表明,微孔体积随着碱金属Cs负载量的增加而逐渐减小,当Cs负载量增加至10 wt%时,样品微孔体积从初始0.105 cm^3/g降至0.063 cm^3/g.NH_3-TPD结果显示,当Cs负载量为1 wt%,酸性催化剂载体上的强酸和弱酸活性位被大量碱性氧化物占据;当负载量超过5 wt%时,所有的酸性位均被覆盖.随后考察负载不同碱金属含量分子筛的羟醛缩合反应性能,发现碱金属氧化物的引入不利于羟醛缩合反应的进行,这主要是由于作为甲醛源的DMM只有在酸中心上才能进行分解产生甲醛,促使羟醛缩合反应顺利进行.当采用DMM为甲醛源时,体系中必须有酸性位存在.同时得知,分子筛HZSM-35中强酸和弱酸均是羟醛缩合反应的有效酸性位,但强酸同时催化原料发生类甲醇制烯烃过程,致使大量烃类副产物生成,产生较重的积炭物种.羟醛缩合反应在含有大量弱酸催化剂上(如γ-Al2O3)也可顺利进行,且具有较高的活性和稳定性. 展开更多
关键词 羟醛缩合反应 甲缩醛 乙酸甲酯 分子筛 酸性
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ZrO_(2)晶相对ZnO/ZrO_(2)+SAPO-34双功能催化剂上合成气制烯烃反应的影响 被引量:1
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作者 刘朝鹏 倪友明 +6 位作者 胡忠攀 傅怡 房旭东 蒋齐可 陈之旸 朱文良 刘中民 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2022年第3期877-884,共8页
烯烃是重要的化工原料,目前主要通过石油催化裂化得到.随着石油资源的消耗以及人们对烯烃需求的日益增长,开发非石油路线制取烯烃势在必行.合成气可以从煤、天然气和生物质等获得,由合成气作为重要的C1平台分子一步制取烯烃(STO)的过程... 烯烃是重要的化工原料,目前主要通过石油催化裂化得到.随着石油资源的消耗以及人们对烯烃需求的日益增长,开发非石油路线制取烯烃势在必行.合成气可以从煤、天然气和生物质等获得,由合成气作为重要的C1平台分子一步制取烯烃(STO)的过程受到了广泛关注.将合成气制甲醇/二甲醚的金属催化剂与甲醇制烯烃的分子筛催化剂耦合得到的混合双功能催化剂,可以使合成气高选择性地转化为烯烃.其中,ZnO/ZrO_(2)金属氧化物催化剂被广泛应于合成气的活化,然而,该金属氧化物结构对混合双功能催化剂上合成气制烯烃反应的影响尚不明确.本文合成了单斜相ZrO_(2)(m-ZrO_(2))和四方相ZrO_(2)(t-ZrO_(2)),并负载ZnO制成催化剂,再将其与SAPO-34分子筛物理混合得到混合双功能催化剂,用于合成气制烯烃反应中.在较优化的条件下,ZnO/m-ZrO_(2)与SAPO-34分子筛组成的双功能催化剂CO转化率为27.9%,低碳烯烃选择性高达80.5%,性能明显优于ZnO/t-ZrO_(2)+SAPO-34双功能催化剂.为研究ZrO_(2)晶相对催化合成气制烯烃反应性能的影响,对ZnO/ZrO_(2)进行红外光谱表征.结果表明,ZnO/m-ZrO_(2)较ZnO/t-ZrO_(2)具有更多的表面羟基和更多的路易斯酸性位点.金属氧化物表面的路易酸主要与催化剂表面不饱和的金属离子有关,而且Zr基催化剂表面羟基有助于缺陷氧的形成,因此,ZnO/m-ZrO_(2)催化剂表面应该具有更高浓度的氧缺陷位.光电子能谱进一步证明了ZnO/m-ZrO_(2)表面有更高浓度的氧缺陷位.另外,Zr基催化剂上表面羟基还有利于CO与其形成羧酸盐物种,在623-673 K条件下的CO原位吸附的红外光谱表明,ZnO/m-ZrO_(2)催化剂上CO吸附的浓度及其表面羧酸盐浓度均明显高于ZnO/t-ZrO_(2)催化剂,这与ZnO/m-ZrO_(2)表现出更好的催化合成气转化性能一致.为了探究该催化剂体系上合成气制烯烃的反应路径,分别对两种晶相的ZnO/ZrO_(2)和相应的双功能催化剂进行了原位红外监测.与CO红外漫反射相比,合成气氛围下金属氧化表面除了存在吸附态的CO和甲酸盐物种,还存在表面甲氧基物种,后者是合成气制甲醇/二甲醚过程重要的中间物种.对合成气制烯烃过程中分子筛上的停留物种进行分析,结果发现,停留物种中含有多甲基苯、多甲基萘等甲醇制烯烃过程中的烃池物种.另外,合成气氛围下双功能催化剂甲氧基信号峰明显弱于金属氧化物表面甲氧基的信号强度,表明STO过程应该是合成气制甲醇/二甲醚与甲醇制烯烃的串联过程.综上所述,在STO反应中,相较于ZnO/t-ZrO_(2)催化剂,ZnO/m-ZrO_(2)催化剂具有更高浓度的表面羟基物种、路易斯酸密度和表面氧缺陷位,从而有利于羧酸盐及甲氧基中间物种的形成,进而提高了混合双功能催化剂催化STO反应性能. 展开更多
关键词 合成气制烯烃 晶相 ZnO/ZrO_(2) SAPO-34 双功能催化剂
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金属氧化物催化剂上合成气转化中羧酸盐物种促进芳烃的生成 被引量:1
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作者 陈之旸 倪友明 +3 位作者 文富利 周子乔 朱文良 刘中民 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2021年第5期835-843,共9页
芳烃是重要的化工原料,目前主要通过石油催化裂化和催化重整制得.随着石油资源的消耗以及芳烃的需求日益增长,开发非石油路线制备芳烃势在必行.因此,从煤、天然气和生物质出发,经合成气一步制芳烃(STA)广受关注.将合成气制甲醇的金属催... 芳烃是重要的化工原料,目前主要通过石油催化裂化和催化重整制得.随着石油资源的消耗以及芳烃的需求日益增长,开发非石油路线制备芳烃势在必行.因此,从煤、天然气和生物质出发,经合成气一步制芳烃(STA)广受关注.将合成气制甲醇的金属催化剂和甲醇制芳烃的分子筛催化剂复合,可以制备双功能催化剂,用于合成气反应可高选择性得到芳烃.然而,关于此过程中芳烃的生成机理仍有争论.目前人们认为,生成芳烃的中间体主要分甲醇和其他含氧物种(乙烯酮,醛类)两种.本文以ZnCrAlO_(x)和H-ZSM-5为模型催化剂,进行合成气制芳烃、甲醇制芳烃和丙烯制芳烃反应,确定了传统的甲醇制芳烃路径不是合成气制芳烃中的主要途径,并通过原位傅里叶变换红外光谱和气相色质谱解释了STA反应中两种活性组分距离越近,芳烃选择性越高的原因,从而提出了在合成气制芳烃过程中芳烃的生成机理.通过比较双功能催化剂上合成气、甲醇以及丙烯的反应性能发现,在甲醇和丙烯转化时,其芳烃选择性远小于合成气转化时的,由此可认为,在合成气制芳烃的路径主要不经由传统的甲醇制芳烃,而是通过烯烃聚合脱氢生成芳烃.红外表征和共进料实验表明,合成气可以在金属催化剂表面生成甲酸盐物种,它可与烯烃反应生成羧酸盐物种,再迁移到分子筛上反应生成芳烃,且羧酸盐物种在分子筛上的芳构化能力要高于丙烯;即使在氢气氛围下,当丙烯的芳构化能力受到氢气极大抑制时,羧酸盐物种仍能高选择性生成芳烃.本文制备了一系列金属催化剂和分子筛物理接近距离不同的双功能催化剂,研究了合成气在双功能催化剂上制芳烃时,金属催化剂和分子筛二者组分的距离对芳烃选择性的影响.随着二者接近距离的增加,芳烃选择性急剧增加;通过GC-MS分析合成气转化时的停留物种,发现随着二者接近距离的增加,羧酸盐物种和甲基环戊烯酮的量明显增加,因此,羧酸盐物种和甲基环戊烯酮物种在生成芳烃中起到了重要的作用.综上所述,我们提出了STA中一条新的芳烃生成路径,并证明了羧酸盐物种是其中重要的中间物种.它经由金属表面的甲酸盐物种和烯烃反应生成,随后迁移到分子筛上生成甲基环戊烯酮物种,再脱水生成芳烃. 展开更多
关键词 羧酸盐 合成气制芳烃 复合催化剂 ZnCrAlO_(x) H-ZSM-5
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Formaldehyde intermediate participating in the conversion of methanol to aromatics over zinc modified H-ZSM-5 被引量:4
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作者 Youming Ni wenliang zhu Zhongmin Liu 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2021年第3期174-178,共5页
Metal-modified H-ZSM-5 has a high selectivity of aromatics in methanol to aromatics(MTA)reaction,which is often attributed to the metal promoting the aromatization of intermediate olefins.However,the effect of methano... Metal-modified H-ZSM-5 has a high selectivity of aromatics in methanol to aromatics(MTA)reaction,which is often attributed to the metal promoting the aromatization of intermediate olefins.However,the effect of methanol dehydrogenation on aromatics formation over these catalysts is rarely studied.Here,we report that HCHO,which is formed by methanol dehydrogenation over Zn/H-ZSM-5 prepared by Zn impregnation,can participate in the synthesis of aromatics.Methanol conversion can produce more aromatics than olefins(propylene or ethylene)conversion over Zn/H-ZSM-5,indicating the conventional MTA pathway including methanol-to-olefins and olefins-to-aromatics is not complete.Moreover,an MTA mechanism including the conventional pathway and the methanol and HCHO coupling pathway is systematically proposed. 展开更多
关键词 METHANOL FORMALDEHYDE AROMATICS Zn H-ZSM-5
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Catalytic activity of Cu/ZnO catalysts mediated by MgO promoter in hydrogenation of methyl acetate to ethanol 被引量:3
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作者 Fang Zhang Zhiyang Chen +3 位作者 Xudong Fang Hongchao Liu Yong Liu wenliang zhu 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2021年第10期203-209,I0006,共8页
Hydrogenation of methyl acetate is a key step in ethanol synthesis from dimethyl ether carbonylation and Cu-based catalysts are widely studied.We report here that the hydrogenation activity of Cu/ZnO catalysts can be ... Hydrogenation of methyl acetate is a key step in ethanol synthesis from dimethyl ether carbonylation and Cu-based catalysts are widely studied.We report here that the hydrogenation activity of Cu/ZnO catalysts can be enhanced by the addition of MgO promoter.The evolution of crystal phases during coprecipitation and the physicochemical properties of calcined and reduced catalysts by X-ray diffraction(XRD),thermogravimetric(TG)-mass spectrometry(MS),Brunauer-Emmett-Teller(BET),transmission electron microscopy(TEM),N_(2)O titration,in situ CO-Fourier transform infrared spectroscopy(FTIR)and H_(2)-temperature programmed reduction(H_(2)-TPR)reveal that the promoter effect likely lies in the presence of Mg^(2+).A proper amount of Mg^(2+)mediates the precipitation process of Cu and Zn,leading to preferable formation of aurichalcite(Cu_(x)Zn_(1-x))5(CO_(3))_(2)(OH)_(6) crystal phase and a small amount of basic carbonates such as hydrozincite Zn_(5)(CO_(3))_(2)(OH)_(6) and malachite Cu_(2) CO_(3)(OH)_(2).The presence of aurichalcite strengthens the interaction between Cu and Zn species,and thus enhances the dispersity of CuO species and helps generation of Cu^(+)species on reduced catalysts.Furthermore,the performance of Cu/ZnO catalysts exhibits an optimal dependence on the Mg loading,i.e.,17.5%.However,too much Mg^(2+)in the precipitation liquid prohibits formation of aurichalcite but enhances formation of basic nitrates,leading to a dramatically reduced hydrogenation activity.These findings may find applications for optimization of other Cu-based catalysts in a wider range of hydrogenation reactions. 展开更多
关键词 Methyl acetate HYDROGENATION Cu/ZnO catalyst MgO promoter Precursor effect Aurichalcite
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Achieving high conversion of syngas to aromatics 被引量:3
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作者 Yi Fu Youming Ni +2 位作者 Zhiyang Chen wenliang zhu Zhongmin Liu 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2022年第3期597-602,I0016,共7页
Realizing high CO conversion and high aromatics selectivity simultaneously in syngas-to-aromatics(STA)reaction is still challenging.Herein,we report a 57.5%CO conversion along with 74%aromatics selectivity over a comp... Realizing high CO conversion and high aromatics selectivity simultaneously in syngas-to-aromatics(STA)reaction is still challenging.Herein,we report a 57.5%CO conversion along with 74%aromatics selectivity over a composite catalyst consisting of Fe/ZnCr_(2)O_(4)(Fe modified ZnCr_(2)O_(4)spinel)oxide and H-ZSM-5 zeolite.Impregnation of only 3 wt%of Fe onto ZnCr_(2)O_(4)can remarkably increase CO conversion without sacrificing the aromatics selectivity.Oxygen vacancy concentration is improved after impregnating Fe.The highly dispersed iron carbide species is formed during the reaction over Fe/ZnCr_(2)O_(4)spinel oxide.The synergistic effect of oxygen vacancy and iron carbide results in a rapid formation of abundant oxygenated intermediate species,which can be continuously transformed to aromatics in H-ZSM-5.This study provides a new insight into the design of highly efficient catalyst for syngas conversion. 展开更多
关键词 SYNGAS AROMATICS Fe/ZnCr_(2)O_(4)oxide H-ZSM-5 zeolite High conversion
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Highly converting syngas to lower olefins over a dual-bed catalyst 被引量:1
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作者 Zhaopeng Liu Youming Ni +2 位作者 Xudong Fang wenliang zhu Zhongmin Liu 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2021年第7期573-576,共4页
Light olefins (C2–C4olefins) are the most important basic carbon-based building blocks, which are mainly produced from the catalytic cracking of naphtha [1–3]. With the rapid depletion of oil reserves and the growin... Light olefins (C2–C4olefins) are the most important basic carbon-based building blocks, which are mainly produced from the catalytic cracking of naphtha [1–3]. With the rapid depletion of oil reserves and the growing demand for lower olefins, there is an urgent need to develop an alternative technique for producing them from non-petroleum resources such as coal, natural gas, or biomass. Currently, coal has been successfully transformed to olefins in China via the combination of the processes of coal-tosyngas, syngas-to-methanol and methanol-to-olefins [4–6]. In order to further improve efficiency and reduce investment, the direct conversion of syngas to olefins has received extensive attention in recent years [7]. 展开更多
关键词 SYNGAS OLEFINS Dual-bed SAPO-34 Dimethyl ether
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Conversion of CO_(2) and H_(2) into propane over InZrO_(x) and SSZ-13 composite catalyst 被引量:1
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作者 Zhaopeng Liu Youming Ni +2 位作者 Tantan Sun wenliang zhu Zhongmin Liu 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2021年第3期111-117,共7页
Direct converting carbon dioxide into hydrocarbon fuels and value-added chemicals would offer a very attractive approach for efficient utilization of CO_(2) as a carbon resource.Although,olefins,aromatics and gasoline... Direct converting carbon dioxide into hydrocarbon fuels and value-added chemicals would offer a very attractive approach for efficient utilization of CO_(2) as a carbon resource.Although,olefins,aromatics and gasoline have been successfully synthesized by CO_(2) hydrogenation,highly selective conversion of CO_(2) and H_(2) into C_(2+)hydrocarbon is still challenging due to a high C-C coupling barrier and inhibiting the production of other long-chain hydrocarbons.Here,we report a composite catalyst made of InZrO_(x) and SSZ-13 molecular sieve(InZrO_(x)+SSZ-13),which exhibits 74.5% propane selectivity at 623 K.The 8-MR micropores and the higher strength of the acid for SSZ-13 benefit the formation of propane.Compared with pure InO_(x) and m-ZrO_(2) the composite oxide InZrO_(x) containing more oxygen vacancies,exhibits to be more readily reduced by H_(2) and easier to adsorb and desorb CO_(2) within the reaction temperature.All those could be beneficial to the activation and conversion of H_(2) and CO_(2).The catalytic performance of InZrO_(x)+SSZ-13 in CO_(2) hydrogenation provides a potential for production of propane. 展开更多
关键词 CO_(2)hydrogenation InZrO_(x)+SSZ-13 PROPANE Oxygen vacancies Acid strength
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Magnetotransport Properties of a Nodal Line Semimetal TiSi 被引量:2
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作者 高默然 何俊宝 +7 位作者 朱文亮 张帅 王欣敏 李婧 麻朝阳 梁慧 任治安 陈根富 《Chinese Physics Letters》 SCIE CAS CSCD 2018年第11期66-69,共4页
We report the magnetoresistance(MR), de Haas-van Alphen(dHvA) effect and Hall effect measurements on a single crystal of TiSi, which is predicted to be a nodal line semimetal. With application of a magnetic field,... We report the magnetoresistance(MR), de Haas-van Alphen(dHvA) effect and Hall effect measurements on a single crystal of TiSi, which is predicted to be a nodal line semimetal. With application of a magnetic field, a metal-to-insulator-like transition in ρ(T) and a nonsaturating MR are observed at low temperatures. The dHvA oscillations reveal a small Fermi-surface pocket with a nontrivial Berry phase. The analysis of the nonlinear Hall resistivity shows that TiSi is a multiband system with low carrier densities and high mobilities. All these results unambiguously prove the existence of Dirac fermions in TiSi. 展开更多
关键词 Magnetotransport Properties of a Nodal Line Semimetal TiSi MR
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A dual-bed catalyst for producing ethylene and propylene from syngas
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作者 Youming Ni Zhaopeng Liu +4 位作者 Peng Tian Zhiyang Chen Yi Fu wenliang zhu Zhongmin Liu 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2022年第3期190-194,I0006,共6页
Ethylene and propylene(C_(2)^(–)3=)are the two most demanded olefin products,which are mainly produced by thermal and catalytic cracking of petroleum-derived hydrocarbons now[1].With the depletion of petroleum resour... Ethylene and propylene(C_(2)^(–)3=)are the two most demanded olefin products,which are mainly produced by thermal and catalytic cracking of petroleum-derived hydrocarbons now[1].With the depletion of petroleum resources,the use of non-petroleum resources such as natural gas,coal,biomass,even CO_(2)etc. 展开更多
关键词 SYNGAS Dual-bed ETHYLENE PROPYLENE SAPO-34
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Superconductivity at the Normal Metal/Dirac Semimetal Cd3As2 Interface
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作者 张帅 王义炎 +4 位作者 麻朝阳 朱文亮 任治安 单磊 陈根富 《Chinese Physics Letters》 SCIE CAS CSCD 2020年第7期107-110,共4页
We investigate the interface between a three-dimensional Dirac semimetal Cd3As2 and a normal metal via softpoint contact spectroscopy measurement.The superconducting gap features were detected below 3.8 K and 7.1 K in... We investigate the interface between a three-dimensional Dirac semimetal Cd3As2 and a normal metal via softpoint contact spectroscopy measurement.The superconducting gap features were detected below 3.8 K and 7.1 K in the case of Cd3As2 single crystals sputter-coated with the Pt and Au films,respectively,in the differential conductance dI/dV-V plots of the point contacts.As the applied magnetic field increased,the drop in the zerobias contact resistance shifted toward lower temperatures.The topologically non-trivial band structure of Cd3As2 is considered to play a crucial role in inducing the superconductivity.Apart from realizing superconductivity in topological materials,our creative approach can be used to investigate possible topological superconductivity and exhibits a high application potential in electronic devices. 展开更多
关键词 SUPERCONDUCTIVITY SUPERCONDUCTIVITY TOPOLOGICAL
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一种在室温附近具有高热电性能的准一维块体材料
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作者 董庆新 项俊森 +15 位作者 王振 李云岫 卢瑞 张特 陈楠 黄奕飞 王义炎 朱文亮 李国栋 赵怀周 郑兴华 张帅 任治安 杨炯 陈根富 孙培杰 《Science Bulletin》 SCIE EI CAS CSCD 2023年第9期920-927,M0004,共9页
在低维材料体系中探索高热电性能是热电材料研究领域的一个重要方向.实际上,近年来所发现的热电材料中的很大一部分,比如Bi_(2)Te_(3),SnSe,Mg_(3)Sb_(2)等,都具有准二维晶体结构.但是,到目前为止对准一维材料的热电研究还非常少见.本... 在低维材料体系中探索高热电性能是热电材料研究领域的一个重要方向.实际上,近年来所发现的热电材料中的很大一部分,比如Bi_(2)Te_(3),SnSe,Mg_(3)Sb_(2)等,都具有准二维晶体结构.但是,到目前为止对准一维材料的热电研究还非常少见.本文报道了一种在室温附近具有高热电性能的准一维块体材料:TLCu_(3)Te_(2).在室温下,该材料沿单晶针状方向具有高达1.3的热电优值;在400 K时,其热电优值甚至可以达到1.5,一定程度超越了目前该温区的商用材料热电性能.通过详细的热电输运实验并结合第一性原理计算,作者发现TlCu_(3)Te_(2)的高热电优值主要起源于饼状费米口袋的高度各向异性准一维电子色散关系带来的大热电功率因子,以及准一维重元素复杂晶格导致的极低热导率.该研究表明准一维块体材料中的单轴性热电效应是一个值得深入探索的热电材料新领地. 展开更多
关键词 热电性能 热电材料 热电优值 热电效应 准一维 第一性原理计算 一维材料 低维材料
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Large transverse thermoelectric figure of merit in a topological Dirac semimetal
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作者 JunSen Xiang SiLe Hu +6 位作者 Meng Lyu wenliang zhu ChaoYang Ma ZiYu Chen Frank Steglich GenFu Chen PeiJie Sun 《Science China(Physics,Mechanics & Astronomy)》 SCIE EI CAS CSCD 2020年第3期82-88,共7页
The Seebeck effect encounters a few fundamental constraints hindering its thermoelectric(TE)conversion efficiency.Most notably,there are the charge compensation of electrons and holes that diminishes this effect,and t... The Seebeck effect encounters a few fundamental constraints hindering its thermoelectric(TE)conversion efficiency.Most notably,there are the charge compensation of electrons and holes that diminishes this effect,and the Wiedemann-Franz(WF)law that makes independent optimization of the corresponding electrical and thermal conductivities impossible.Here,we demonstrate that in the topological Dirac semimetal Cd3As2 the Nernst effect,i.e.,the transverse counterpart of the Seebeck effect,can generate a large TE figure of merit zNT.At room temperature,zNT≈0.5 in a small field of 2 T and it significantly surmounts its longitudinal counterpart for any field.A large Nernst effect is generically expected in topological semimetals,benefiting from both the bipolar transport of compensated electrons and holes and their high mobilities.In this case,heat and charge transport are orthogonal,i.e.,not intertwined by the WF law anymore.More importantly,further optimization of zNT by tuning the Fermi level to the Dirac node can be anticipated due to not only the enhanced bipolar transport,but also the anomalous Nernst effect arising from a pronounced Berry curvature.A combination of the topologically trivial and nontrivial advantages promises to open a new avenue towards high-efficient transverse thermoelectricity. 展开更多
关键词 DIRAC SEMIMETAL Cd3As2 Nernst effect TRANSVERSE THERMOELECTRICITY
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High-throughput sequencing detection and ensartinib treatment of lung cancer harboring NTRK1 fusion
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作者 Zhengbo Song Chunwei Xu +10 位作者 Xingxiang Pu Youcai zhu Wenxian Wang Xingliang Li Yanqiu Gao wenliang zhu Yunwei He Lin Wu Li Mao Li Chen Ming Chen 《Cancer Communications》 SCIE 2021年第2期192-196,共5页
Dear Editor,Although fusion events involving neurotrophic receptor tyrosine kinase 1,2,and 3 genes(NTRK1,NTRK2,and NTRK3,encoding TRKA/B/C respectively)were found in diverse tumor types,only 0.1%-0.3%of lung cancer pa... Dear Editor,Although fusion events involving neurotrophic receptor tyrosine kinase 1,2,and 3 genes(NTRK1,NTRK2,and NTRK3,encoding TRKA/B/C respectively)were found in diverse tumor types,only 0.1%-0.3%of lung cancer patients harbor an NTRK(and mostly NTRK1)fusion as the primary oncogenic event[1].Such low prevalence may be partially due to the limited availability of first-line assays for detecting rare fusion events[2].Immunohistochemistry is limited by sensitivity and variable tissue background,and fluorescence in-situ hybridization falls short of elucidating functional significance such as the identity of the partner or structure of the transcript.While DNA next-generation sequencing(NGS)is suitable for mutation calling(single nucleotide variation[SNV]and insertion-or-deletion[indel]),and RNA NGS is particularly effective in detecting fusions[3],routinely performing these two assays together is labor-intensive.As a solution,we have developed a single NGS assay(PANO-Seq)for unified RNA/DNA target enrichment library preparation[4],which takes about 12 hours and $10 to prepare. 展开更多
关键词 ROUTINE HARBOR TREATMENT
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Small tracking error correction for moving targets of intelligent electro-optical detection systems
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作者 Cheng SHEN Zhijie WEN +2 位作者 wenliang zhu Dapeng FAN Mingyuan LING 《Frontiers of Mechanical Engineering》 SCIE 2024年第2期29-44,共16页
Small tracking error correction for electro-optical systems is essential to improve the tracking precision of future mechanical and defense technology.Aerial threats,such as“low,slow,and small(LSS)”moving targets,po... Small tracking error correction for electro-optical systems is essential to improve the tracking precision of future mechanical and defense technology.Aerial threats,such as“low,slow,and small(LSS)”moving targets,pose increasing challenges to society.The core goal of this work is to address the issues,such as small tracking error correction and aiming control,of electro-optical detection systems by using mechatronics drive modeling,composite velocity–image stability control,and improved interpolation filter design.A tracking controller delay prediction method for moving targets is proposed based on the Euler transformation model of a two-axis,two-gimbal cantilever beam coaxial configuration.Small tracking error formation is analyzed in detail to reveal the scientific mechanism of composite control between the tracking controller’s feedback and the motor’s velocity–stability loop.An improved segmental interpolation filtering algorithm is established by combining line of sight(LOS)position correction and multivariable typical tracking fault diagnosis.Then,a platform with 2 degrees of freedom is used to test the system.An LSS moving target shooting object with a tracking distance of S=100 m,target board area of A=1 m^(2),and target linear velocity of v=5 m/s is simulated.Results show that the optimal method’s distribution probability of the tracking error in a circle with a radius of 1 mrad is 66.7%,and that of the traditional method is 41.6%.Compared with the LOS shooting accuracy of the traditional method,the LOS shooting accuracy of the optimized method is improved by 37.6%. 展开更多
关键词 electro-optical detection system small tracking error moving target visual servo aiming contro
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