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Catalytic Hydrogenolysis of HMF to DMF over N-doped Molybdenum Carbide Catalyst 掺杂 N 的碳化钼催化剂催化加氢分解 HMF 至 DMF
IF 2.3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2024-06-24 DOI: 10.1007/s10562-024-04757-0
Peng Rui, Wenfei Huang, Qian Xu, Han Lu, Tongqi Ye, Xin Yao, Yuewen Ye, Rulong Zhou

The effect of organic precursors on catalysts was studied and the preparation of catalyst and reaction conditions were optimized. A 91% selectivity of 2,5-dimethylfuran (DMF) from the hydrogenolysis of 5-hydroxymethylfurfural (HMF) was obtained on a Mo monometallic catalyst, in which nitrogen doping played a key role. Density functional theory (DFT) shows that Mo sites with N, O and C coordination have moderate adsorption strength of HMF and H2 and lower energy barrier of key steps compared with pure molybdenum nitride, molybdenum carbide and molybdenum oxide, which may be conducive to catalytic hydrogenolysis of HMF.

Graphical Abstract

研究了有机前体对催化剂的影响,并对催化剂的制备和反应条件进行了优化。在掺氮起关键作用的钼单金属催化剂上,5-羟甲基呋喃(HMF)氢解生成 2,5 二甲基呋喃(DMF)的选择性达到 91%。密度泛函理论(DFT)表明,与纯氮化钼、碳化钼和氧化钼相比,具有 N、O 和 C 配位的钼位点对 HMF 和 H2 的吸附强度适中,关键步骤的能垒较低,这可能有利于催化 HMF 的氢解。
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引用次数: 0
Visible Light-Responsive AlFeO3@g-C3N4 Heterojunction for Efficient Degradation of Organic Wastewater 用于高效降解有机废水的可见光响应型 AlFeO3@g-C3N4 异质结
IF 2.3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2024-06-22 DOI: 10.1007/s10562-024-04751-6
Zixuan Li, Rui Mu, Wei Zhang, Xue Lin, Qi Cui, Di Gu

A Z-type AlFeO3@g-C3N4 photocatalyst was successfully prepared via sol-gel and high-temperature polymerization. The morphology, structure, and composition of the catalysts were analyzed by X-ray diffraction, scanning electron microscopy, and transmission electron microscopy. The photocatalytic performance was evaluated by nitrobenzene degradation experiments and electrochemical station, comparing with single g-C3N4 and AlFeO3. Optimizing AlFeO3 precursor content in the composite yielded 1.6 and 1.8-fold higher degradation rates than single g-C3N4 and AlFeO3, respectively. Furthermore, in comparison to other ratios of AlFeO3@g-C3N4 composites, AF-CN-100, which exhibited the best degrading performance, had the smallest impedance, the strongest transient photocurrent response strength, and the strongest redox capacity. The heterojunction produced between AlFeO3 and g-C3N4 was a Z-type heterojunction, as revealed by investigations on energy band structure and mechanism. This heterojunction substantially improved the separation efficiency of photogenerated electrons and holes and increased the photocatalytic activity of the composites.

摘要 通过溶胶-凝胶法和高温聚合法成功制备了Z型AlFeO3@g-C3N4光催化剂。采用 X 射线衍射、扫描电子显微镜和透射电子显微镜分析了催化剂的形貌、结构和组成。通过硝基苯降解实验和电化学站评估了催化剂的光催化性能,并与单一 g-C3N4 和 AlFeO3 进行了比较。通过优化复合材料中 AlFeO3 前驱体的含量,降解率分别比单一 g-C3N4 和 AlFeO3 高出 1.6 倍和 1.8 倍。此外,与其他比例的 AlFeO3@g-C3N4 复合材料相比,降解性能最好的 AF-CN-100 阻抗最小,瞬态光电流响应强度最大,氧化还原能力最强。能带结构和机理研究表明,AlFeO3 和 g-C3N4 之间产生的异质结为 Z 型异质结。这种异质结大大提高了光生电子和空穴的分离效率,提高了复合材料的光催化活性。
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引用次数: 0
CuO Decorated Magnetic Reduced Graphene Oxide Catalyzed Cross-Dehydrogenative Coupling of Thiols and Alkylbenzenes 氧化铜装饰的磁性还原石墨烯氧化物催化硫醇与烷基苯的交叉脱氢偶联反应
IF 2.3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2024-06-22 DOI: 10.1007/s10562-024-04761-4
Marzieh Rousta, Dariush Khalili, Edris Ebrahimi, Ali Khoy

An efficient C-S cross-dehydrogenative coupling (CDC) has been achieved using rGO/Fe3O4-CuO as a robust nanocatalyst in the presence of TBHP and SDS as a surfactant for the thioesterification of cost-effective methylarenes with thiols in water. This heterogeneous Cu catalyst exhibited excellent performance and recyclability in the synthesis of thioesters without the assistance of any directing group.

Graphical Abstract

Magnetic reduced graphene oxide supported CuO catalyzed cross-dehydrogenative coupling of thiols and alkylbenzenes: Direct access to thioesters.

利用rGO/Fe3O4-CuO作为强效纳米催化剂,在TBHP和SDS作为表面活性剂存在下,实现了高效的C-S交叉脱氢偶联(CDC),用于在水中对具有成本效益的甲基烯与硫醇进行硫酯化反应。这种异相铜催化剂在合成硫代酯类化合物时表现出优异的性能和可回收性,无需任何定向基团的辅助:直接获得硫代酯。
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引用次数: 0
Preparation of Thermosensitive Polymer Immobilized Horseradish Peroxidase and its Application in Catalytic Degradation of Phenol 热敏聚合物固定化辣根过氧化物酶的制备及其在催化降解苯酚中的应用
IF 2.3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2024-06-22 DOI: 10.1007/s10562-024-04730-x
Yuanyuan Li, Yuanyuan Chen, Tongyu Li, Yongqing Song, Jiacong Wu, Juan Han, Yun Wang

The immobilized horseradish peroxidase (P1-HRP) was prepared based on the affinity interaction between the phenylborate group in mVBA-b-p (AAm co AN) polymer (P1) and the adjacent dihydroxy group in horseradish peroxidase (HRP). The immobilization conditions of P1-HRP were optimized. Under the conditions of P1 concentration of 20 mg/mL, pH 8, temperature of 50 ℃, and immobilization time of 2 h, the HRP was immobilized to obtain the optimal immobilization amount (84.7 mg/g). The successful preparation of P1-HRP was demonstrated through characterizations such as laser scanning confocal microscopy (LCSM), scanning electron microscope (SEM), dynamic light scattering (DLS) and thermogravimetric analyzer (TGA). P1-HRP exhibited excellent pH stability, thermal stability and storage stability compared to the free horseradish peroxidase. P1-HRP had shown good application value in the degradation of phenol pollutants. After 10 repetitions of phenol degradation, the relative enzyme activity of P1-HRP could still be retained by 55.62%, indicating its good reusability. The optimal conditions for the catalytic degradation of phenol by P1-HRP were optimized. After catalytic degradation of phenol for 60 min under the same conditions, the degradation rate of P1-HRP (92.33%) was higher than that of free horseradish peroxidase (85.32%).

Graphical abstract

根据 mVBA-b-p (AAm co AN) 聚合物(P1)中的苯基硼酸酯基团与辣根过氧化物酶(HRP)中相邻的二羟基之间的亲和力作用,制备了固定化辣根过氧化物酶(P1-HRP)。对 P1-HRP 的固定条件进行了优化。在 P1 浓度为 20 mg/mL、pH 值为 8、温度为 50 ℃、固定时间为 2 h 的条件下,固定 HRP 得到了最佳固定量(84.7 mg/g)。通过激光扫描共聚焦显微镜(LCSM)、扫描电子显微镜(SEM)、动态光散射(DLS)和热重分析仪(TGA)等表征,证明了 P1-HRP 的成功制备。与游离辣根过氧化物酶相比,P1-HRP 具有优异的 pH 稳定性、热稳定性和储存稳定性。P1-HRP 在降解苯酚污染物方面具有良好的应用价值。在重复降解苯酚 10 次后,P1-HRP 的相对酶活性仍能保持 55.62%,表明其具有良好的重复使用性。对 P1-HRP 催化降解苯酚的最佳条件进行了优化。在相同条件下催化降解苯酚 60 分钟后,P1-HRP 的降解率(92.33%)高于游离辣根过氧化物酶的降解率(85.32%)。
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引用次数: 0
Effect of Ni-W Morphology on the Catalytic Ethylbenzene Hydrogenation Ni-W 形态对催化乙苯加氢的影响
IF 2.3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2024-06-21 DOI: 10.1007/s10562-024-04740-9
Nan Zheng, Yunyun Dong, Juan Xu, Wenqiang Lai

Ni-W catalysts find extensive application in catalysis; however, the impact of diverse morphologies on their catalytic activity remains a relatively unexplored area. Using hydrothermal/solvothermal synthesis methods, we successfully synthesized Ni-W catalysts with various morphologies, including sheet-like, sphere-like, rod-like, flower-like, and particulate-like structures. Comprehensive investigations into the influence of morphology on the catalytic activity of these Ni-W catalysts were conducted, employing techniques such as SEM, XRD, XPS, TG-DTG, BET, H2-TPR, and H2-TPD. Remarkably, the flower-like Ni-W catalyst displayed exceptional catalytic properties in ethylbenzene hydrogenation, exhibiting not only high hydrogenation activity but also superior sulfur resistance. Consequently, the flower-like Ni-W catalyst holds great potential for applications in industrial catalysis.

Graphical Abstract

镍-钨催化剂在催化领域有着广泛的应用,然而,不同形态对其催化活性的影响仍是一个相对未开发的领域。我们采用水热/溶热合成方法,成功合成了各种形态的 Ni-W 催化剂,包括片状、球状、棒状、花朵状和颗粒状结构。我们采用 SEM、XRD、XPS、TG-DTG、BET、H2-TPR 和 H2-TPD 等技术全面研究了形态对这些 Ni-W 催化剂催化活性的影响。值得注意的是,花状 Ni-W 催化剂在乙苯加氢过程中表现出优异的催化性能,不仅具有很高的加氢活性,而且还具有优异的抗硫性能。因此,花状 Ni-W 催化剂在工业催化领域具有巨大的应用潜力。
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引用次数: 0
Synthesis of Green Heterogeneous Bifunctional Zeolite-A/Biochar Catalyst for the Production of Biodiesel from Waste Cooking Oil 利用废食用油生产生物柴油的绿色异构双功能沸石-A/生物炭催化剂的合成
IF 2.3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2024-06-21 DOI: 10.1007/s10562-024-04746-3
Tessema Derbe, Enyew. A Zereffa, Taju Sani, Teketel Girma

Green heterogeneous bifunctional catalyst is sustainable for the production of biodiesel owning to its reusability, eco-friendly, and bifunctionality. In this work, a green heterogeneous bifunctional Zeolite-A/Biochar (Z-A/BC) catalyst was synthesized for the production of biodiesel from waste cooking oil (WCO) through one-pot esterification-transesterification reaction. The functional group, elemental composition, crystallographic structure, and morphology of the synthesized catalyst were characterized using FT-IR, EDX, XRD, and SEM, respectively. Furthermore, the catalytic proficiency of the synthesized catalyst was tested by optimizing methanol to oil ratio, catalyst amount, temperature, and reaction time. The maximum biodiesel yield (86.22%) was achieved at 2.5% wt. of catalyst amount, 10:1 of methanol to oil molar ratio, 70 °C of reaction temperature, and 240 min of reaction time. The synthesized Z-A/BC catalyst showed apparent catalytic efficiency than its parent materials Z-A (69.42%) and BC (74.27%). The recyclability of Z-A/BC catalyst was also found to be 86.22, 82.98, 79.08, 62.87, and 76.84% for 1st, 2nd, 3rd, 4th, and 5th cycles, sequentially which is cost effective. Furthermore, the physicochemical properties such as density, ash content, FFA, acid value, saponification value, and kinematic viscosity of the produced biodiesel were analyzed by comparing with standards. These results showed good agreement with ASTM and EN14214 biodiesel standards. Therefore, the produced biodiesel using heterogeneous bifunctional Z-A/BC catalyst from WCO could be used as an alternative engine fuel with/without blending with commercial diesel.

Graphical Abstract

绿色异构双功能催化剂具有可重复使用性、生态友好性和双功能性,可持续用于生物柴油的生产。本研究合成了一种绿色异相双功能沸石-A/生物炭(Z-A/BC)催化剂,用于利用废弃食用油(WCO)通过一锅酯化-酯交换反应生产生物柴油。利用 FT-IR、EDX、XRD 和 SEM 分别对合成催化剂的官能团、元素组成、晶体结构和形貌进行了表征。此外,通过优化甲醇与油的比例、催化剂用量、温度和反应时间,测试了合成催化剂的催化能力。在催化剂用量为 2.5%、甲醇与油的摩尔比为 10:1、反应温度为 70 °C、反应时间为 240 分钟的条件下,生物柴油产率达到最大值(86.22%)。合成的 Z-A/BC 催化剂的催化效率明显高于其母体材料 Z-A(69.42%)和 BC(74.27%)。研究还发现,Z-A/BC 催化剂在第一、第二、第三、第四和第五次循环中的可回收性依次为 86.22%、82.98%、79.08%、62.87% 和 76.84%,具有很高的成本效益。此外,通过与标准进行比较,分析了所生产生物柴油的物理化学特性,如密度、灰分含量、FFA、酸值、皂化值和运动粘度。这些结果表明与 ASTM 和 EN14214 生物柴油标准非常一致。因此,使用 WCO 的异构双功能 Z-A/BC 催化剂生产的生物柴油可用作替代发动机燃料,与商用柴油混合使用或不混合使用。
{"title":"Synthesis of Green Heterogeneous Bifunctional Zeolite-A/Biochar Catalyst for the Production of Biodiesel from Waste Cooking Oil","authors":"Tessema Derbe,&nbsp;Enyew. A Zereffa,&nbsp;Taju Sani,&nbsp;Teketel Girma","doi":"10.1007/s10562-024-04746-3","DOIUrl":"10.1007/s10562-024-04746-3","url":null,"abstract":"<div><p>Green heterogeneous bifunctional catalyst is sustainable for the production of biodiesel owning to its reusability, eco-friendly, and bifunctionality. In this work, a green heterogeneous bifunctional Zeolite-A/Biochar (Z-A/BC) catalyst was synthesized for the production of biodiesel from waste cooking oil (WCO) through one-pot esterification-transesterification reaction. The functional group, elemental composition, crystallographic structure, and morphology of the synthesized catalyst were characterized using FT-IR, EDX, XRD, and SEM, respectively. Furthermore, the catalytic proficiency of the synthesized catalyst was tested by optimizing methanol to oil ratio, catalyst amount, temperature, and reaction time. The maximum biodiesel yield (86.22%) was achieved at 2.5% wt. of catalyst amount, 10:1 of methanol to oil molar ratio, 70 °C of reaction temperature, and 240 min of reaction time. The synthesized Z-A/BC catalyst showed apparent catalytic efficiency than its parent materials Z-A (69.42%) and BC (74.27%). The recyclability of Z-A/BC catalyst was also found to be 86.22, 82.98, 79.08, 62.87, and 76.84% for 1<sup>st</sup>, 2<sup>nd</sup>, 3<sup>rd</sup>, 4<sup>th</sup>, and 5<sup>th</sup> cycles, sequentially which is cost effective. Furthermore, the physicochemical properties such as density, ash content, FFA, acid value, saponification value, and kinematic viscosity of the produced biodiesel were analyzed by comparing with standards. These results showed good agreement with ASTM and EN14214 biodiesel standards. Therefore, the produced biodiesel using heterogeneous bifunctional Z-A/BC catalyst from WCO could be used as an alternative engine fuel with/without blending with commercial diesel.</p><h3>Graphical Abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2024-06-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141511566","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
One-pot Hydrothermal Synthesis of Bifunctional Co/Mo-rGO efficient Electrocatalyst for HER/OER in Water Splitting 一锅水热法合成双功能 Co/Mo-rGO 高效电催化剂,用于水分离中的 HER/OER
IF 2.3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2024-06-21 DOI: 10.1007/s10562-024-04723-w
Lishuang Zhao, Siyan Liu, Liguo Wei, Huiyi He, Bo Jiang, Zhaoshun Zhan, Jing Wang, Xuewei Li, Wentao Gou

Fabrication of highly efficient and earth-abundant bifunctional electrocatalyst to accelerate the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) are critical for overall water splitting. In this work, bimetallic Co/Mo oxides modified reduced graphene oxide (rGO) was synthesized using a simple one-pot hydrothermal method, which significantly improved the electrocatalytic activity in both HER and OER. Under the optimal conditions, the double layer capacitance of rGO modified by Co/Mo bimetal is 78.08 mF cm−2. The overpotential required for HER to reach -10 mA cm−2 current density is 488 mV, the dynamic Tafel slope is 126 mV dec−1. The overpotential required for OER to reach 10 mA cm−2 current density is 420 mV, the slope of kinetic Tafel is 169 mV dec−1. This work provides a new prospect for the rational design and fabrication of efficient HER/OER bifunctional electrocatalysts in electrochemical energy device application.

Graphical Abstract

制备高效且富含土的双功能电催化剂以加速氢进化反应(HER)和氧进化反应(OER)对整个水分离过程至关重要。本研究采用简单的一锅水热法合成了双金属 Co/Mo 氧化物修饰的还原氧化石墨烯(rGO),显著提高了 HER 和 OER 的电催化活性。在最佳条件下,经 Co/Mo 双金属修饰的 rGO 的双层电容为 78.08 mF cm-2。HER 达到 -10 mA cm-2 电流密度所需的过电位为 488 mV,动态塔菲尔斜率为 126 mV dec-1。OER 达到 10 mA cm-2 电流密度所需的过电位为 420 mV,动力学塔菲尔斜率为 169 mV dec-1。这项工作为合理设计和制备高效的 HER/OER 双功能电催化剂在电化学能源装置中的应用提供了新的前景。
{"title":"One-pot Hydrothermal Synthesis of Bifunctional Co/Mo-rGO efficient Electrocatalyst for HER/OER in Water Splitting","authors":"Lishuang Zhao,&nbsp;Siyan Liu,&nbsp;Liguo Wei,&nbsp;Huiyi He,&nbsp;Bo Jiang,&nbsp;Zhaoshun Zhan,&nbsp;Jing Wang,&nbsp;Xuewei Li,&nbsp;Wentao Gou","doi":"10.1007/s10562-024-04723-w","DOIUrl":"10.1007/s10562-024-04723-w","url":null,"abstract":"<div><p>Fabrication of highly efficient and earth-abundant bifunctional electrocatalyst to accelerate the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) are critical for overall water splitting. In this work, bimetallic Co/Mo oxides modified reduced graphene oxide (rGO) was synthesized using a simple one-pot hydrothermal method, which significantly improved the electrocatalytic activity in both HER and OER. Under the optimal conditions, the double layer capacitance of rGO modified by Co/Mo bimetal is 78.08 mF cm<sup>−2</sup>. The overpotential required for HER to reach -10 mA cm<sup>−2</sup> current density is 488 mV, the dynamic Tafel slope is 126 mV dec<sup>−1</sup>. The overpotential required for OER to reach 10 mA cm<sup>−2</sup> current density is 420 mV, the slope of kinetic Tafel is 169 mV dec<sup>−1</sup>. This work provides a new prospect for the rational design and fabrication of efficient HER/OER bifunctional electrocatalysts in electrochemical energy device application.</p><h3>Graphical Abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2024-06-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141511590","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Vapor Phase Cross Ketonization of Pivalic Acid with Acetic Acid to Prepare Pinacolone Over Mg-Zr Mixed Oxide Catalysts 在 Mg-Zr 混合氧化物催化剂上气相交叉酮化特戊酸与乙酸以制备频哪酮
IF 2.3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2024-06-21 DOI: 10.1007/s10562-024-04752-5
P. Mahesh Kumar, Y. Nagesh, G. Mallikarjun, N. Lingaiah

A sequence of MgO-ZrO2 mixed oxides with varying their ratios were synthesized by adopting co-precipitation method. These catalysts characteristics were deduced from different spectroscopic methods and used for vapor phase cross-ketonization of pivalic acid with acetic acid to produce pinacolone at atmospheric pressure. The characterization results indicated that at a high ZrO2 molar ratio, MgxZr1-xO2-x mixed oxide phase is formed, and it accounted for the presence of strong basic sites. MgO-ZrO2 mixed oxides ketonization activity is superior to individual oxides and the overall activity mainly depended on their molar ratio, calcination temperature, and presence of mixed oxide phase. The basicity of the MgO-ZrO2 mixed oxide catalyst is responsible for the high conversion of pivalic acid. The ketonization reaction is carried under different reaction parameters and optimized conditions were established. The catalysts are showed stability during the time on stream analysis.

Graphical Abstract

采用共沉淀法合成了一系列不同比例的 MgO-ZrO2 混合氧化物。通过不同的光谱方法推断了这些催化剂的特性,并将其用于在常压下对特戊酸与乙酸进行气相交叉酮化反应,生成频哪酮。表征结果表明,在较高的 ZrO2 摩尔比下,会形成 MgxZr1-xO2-x 混合氧化物相,这也是强碱性位点存在的原因。MgO-ZrO2 混合氧化物的酮化活性优于单个氧化物,整体活性主要取决于它们的摩尔比、煅烧温度和混合氧化物相的存在。MgO-ZrO2 混合氧化物催化剂的碱性是特戊酸高转化率的原因。酮化反应在不同的反应参数下进行,并建立了优化条件。催化剂在流式分析过程中表现出稳定性。
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引用次数: 0
Comparative Study of Different Mesostructured Silica-supported Nano-iron Catalysts for Fischer–Tropsch Synthesis 用于费托合成的不同介质结构二氧化硅支撑纳米铁催化剂的比较研究
IF 2.3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2024-06-21 DOI: 10.1007/s10562-024-04764-1
Yaqian Liu, Feng Wu, Zhixiong You, Jinjun Li

Fischer-Tropsch synthesis (FTS) converts syngas into multi-carbon products, whose distribution is highly dependent on the catalyst structure. Here, nano-iron catalysts with different silica supports were prepared, and their activities and durability for Fischer-Tropsch to olefins (FTO) process were investigated. Fe/KCC-1 demonstrated the best FTO catalytic selectivity of 25.0% for C2–4= and an olefin-to-paraffin ratio of 1.68. Its open pore structure allowed primary olefins to escape quickly from the catalyst surface, lowering the probability for secondary reactions. However, its durability was lower than Fe/SBA-15 due to coke formation, pore structure collapse and Fe particle agglomeration. The thermal stability of SBA-15 resulted in its better durability, and the encapsulated Fe particles inside the cylindrical mesopores also allowed better resistance to sintering. However, the less open structure of Fe/SBA-15 led to longer residence time for the primary olefins and increased possibility for secondary reactions, causing undesired chain growth.

摘要费托合成(FTS)将合成气转化为多碳产品,其分布与催化剂结构密切相关。本文制备了具有不同二氧化硅载体的纳米铁催化剂,并研究了它们在费托合成烯烃(FTO)过程中的活性和耐久性。Fe/KCC-1 对 C2-4= 的 FTO 催化选择性最好,为 25.0%,烯烃与石蜡的比率为 1.68。其开放式孔隙结构允许初级烯烃迅速从催化剂表面逸出,从而降低了发生二次反应的几率。然而,由于焦炭形成、孔隙结构坍塌和铁颗粒团聚,其耐久性低于 Fe/SBA-15。SBA-15 的热稳定性使其具有更好的耐久性,圆柱形中孔内包裹的铁颗粒也使其具有更好的抗烧结性。然而,Fe/SBA-15 的开放结构较少,导致初级烯烃的停留时间延长,增加了发生二次反应的可能性,从而引起了不希望的链增长。
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引用次数: 0
Superhydrophilic Self-supported Perovskite Oxides for Oxygen Evolution Reactions in Oilfield Wastewater 用于油田废水中氧进化反应的超亲水性自支撑 Perovskite 氧化物
IF 2.3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2024-06-20 DOI: 10.1007/s10562-024-04753-4
Jianzhao Cao, Salman Riaz, Zhaoxiang Qi, Ke Zhao, Ying Qi, Peng Wei, Yahong Xie

Developing highly efficient catalysts for oxygen evolution reactions (OER) in complex water environments is crucial for promoting the photovoltaic electrolysis of water splitting for hydrogen production in arid areas. However, traditional catalysts often exhibit limitations in terms of reaction kinetics and electrode corrosion resistance. In this work, we successfully prepared a self-supporting perovskite complex oxide La0.7Sr0.3CoO3-δ/NF (LSC/NF) catalyst by means of simple hydrothermal synthesis combined with programmed annealing, and successfully applied to OER reaction in oilfield wastewater. In alkaline oilfield wastewater, at a current density of 10 mA cm−2, LSC/NF requires only 411 mV of overpotential, which is lower than that of LSC (493 mV) and traditional catalyst RuO2 (451 mV), suggesting a high OER catalytic activity. The good electrocatalytic activity can be attributed to its superhydrophilicity, increased electrochemical active surface area, faster reaction kinetics and higher oxygen vacancy concentration. This research offers valuable new insights for the development of OER electrocatalysts with high catalytic activity in complex water systems in arid areas.

Graphical Abstract

A self-supporting perovskite oxide catalyst La0.7Sr0.3CoO3-δ/NF was synthesized by a simple process combining hydrothermal and annealing. The growth of perovskite oxide nanosheets directly on the conductive nickel foam matrix gives the catalyst a strong hydrophilicity and significantly expands its electrochemical active surface area, thus enhancing the OER activity of LSC/NF in oilfield wastewater.

开发用于复杂水环境中氧进化反应(OER)的高效催化剂,对于促进干旱地区光伏电解水分裂制氢至关重要。然而,传统催化剂往往在反应动力学和电极耐腐蚀性方面表现出局限性。在这项工作中,我们通过简单的水热合成结合程序退火,成功制备了自支撑包晶复合氧化物 La0.7Sr0.3CoO3-δ/NF (LSC/NF)催化剂,并成功应用于油田废水中的 OER 反应。在碱性油田废水中,当电流密度为 10 mA cm-2 时,LSC/NF 只需要 411 mV 的过电位,低于 LSC(493 mV)和传统催化剂 RuO2(451 mV),这表明其具有很高的 OER 催化活性。良好的电催化活性可归因于它的超亲水性、更大的电化学活性表面积、更快的反应动力学和更高的氧空位浓度。该研究为在干旱地区的复杂水系统中开发具有高催化活性的 OER 电催化剂提供了有价值的新见解。 图解 摘要 采用水热法和退火法相结合的简单工艺合成了自支撑包晶氧化物催化剂 La0.7Sr0.3CoO3-δ/NF。过闪石氧化物纳米片直接生长在导电泡沫镍基体上,使催化剂具有很强的亲水性,并显著扩大了其电化学活性表面积,从而提高了 LSC/NF 在油田废水中的 OER 活性。
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引用次数: 0
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Catalysis Letters
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