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Synthesis of FeOx-supported nano-silver catalyst and the mechanism of electrocatalytic epoxidation of propylene feox负载纳米银催化剂的合成及丙烯电催化环氧化机理
Q3 Energy Pub Date : 2025-10-01 DOI: 10.1016/S1872-5813(25)60546-9
Dengwen PI , Xiaobo YANG , Xuning LI
The electrochemical oxidation of propylene offers a promising green process route for propylene oxide (PO) synthesis. However, due to complex by-products and low yields, its development has been hampered. Therefore, it is crucial to explore the reaction mechanism of propylene epoxidation to guide the targeted design of efficient catalysts. In this work, FeOx-supported nano-silver catalysts (Ag-Fe2O3) were designed to achieve the efficient utilization of noble metal Ag to use for the electro-catalytic epoxidation of propylene, and the Ag loading in Fe2O3 was regulated by a hydrothermal method combined with a co-precipitation method. When the loading of Ag in Fe2O3 is 1.82%, it effectively enhanced the efficiency of the propylene epoxidation reaction, with the Faraday efficiency of 26.2% for PO, and its performance was superior to that of Fe2O3 and other samples with different loadings. The bifunctional mechanism was clarified by in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS), where propylene was adsorbed on the surface of Fe2O3 and the nano-Ag sites promoted the generation of reactive oxygen species such as *O and *OOH. This work elucidates synergistic catalytic effect between metal and support, provides new mechanistic insights for the electrochemical epoxidation of propylene, and offers possible theoretical guidance for the design of high-performance catalysts.
丙烯的电化学氧化为合成环氧丙烷(PO)提供了一条很有前途的绿色工艺路线。但由于其副产品复杂、产率低,制约了其发展。因此,探索丙烯环氧化反应机理,指导有针对性地设计高效催化剂至关重要。本文设计了feox负载的纳米银催化剂(Ag-Fe2O3),实现了贵金属Ag在丙烯电催化环氧化反应中的高效利用,并采用水热法结合共沉淀法调节了Fe2O3中Ag的负载。Fe2O3中Ag的掺量为1.82%时,能有效提高丙烯环氧化反应的效率,PO的法拉第效率为26.2%,性能优于Fe2O3和其他不同掺量样品。通过原位衰减全反射表面增强红外吸收光谱(ATR-SEIRAS)研究了双功能机理,其中丙烯吸附在Fe2O3表面,纳米ag位点促进了*O和*OOH等活性氧的生成。本研究阐明了金属与载体之间的协同催化作用,为丙烯的电化学环氧化反应提供了新的机理认识,并为高性能催化剂的设计提供了可能的理论指导。
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引用次数: 0
Progress in the modulation strategies of heterogeneous catalysts for ammonia synthesis by nitric oxide reduction 一氧化氮还原合成氨的多相催化剂调控策略研究进展
Q3 Energy Pub Date : 2025-10-01 DOI: 10.1016/S1872-5813(25)60570-6
Na LI , Yanyan YANG , Song YANG , Zhongliang YU
Nitric oxide (NO) is one of the most hazardous pollutants in the atmosphere, posing a serious threat to human health and ecological environment. Traditional treatment methods show high energy consumption and poor economics. New technologies for the efficient conversion of NO to ammonia (NH3), which are in line with green sustainability, have received widespread attention. However, existing catalysts suffer from numerous problems like their insufficient reactivity, low selectivity, and poor stability. Numerous studies have found that modulation of the catalyst structure can improve these problems. Therefore, this paper reviews the research progress in the modulation strategies of catalysts for the synthesis of NH3 by reduction NO, and discusses the possible measures that can enhance the catalytic activity, such as energy band modification and electronic modulation, vacancy engineering, elemental doping, and amorphous engineering modulation, etc., as well as the critical factors that influence the catalytic selectivity to NH3, such as the hydrogen bonding effect and single-atom/highly dispersed sites, etc. In addition, the metal-to-metal/support interactions and the confinement engineering, nano-engineering, and other strategies for strengthening the catalyst stability are also analyzed. Finally, this paper summarizes the challenges faced by this technology in practice and looks into the prospect of this technology in future application.
一氧化氮(NO)是大气中危害最大的污染物之一,对人类健康和生态环境构成严重威胁。传统的处理方法能耗高,经济性差。符合绿色可持续性的NO高效转化为氨(NH3)的新技术受到了广泛关注。然而,现有的催化剂存在反应性不足、选择性低、稳定性差等问题。大量研究发现,调整催化剂结构可以改善这些问题。因此,本文综述了还原NO合成NH3催化剂调制策略的研究进展,讨论了提高催化活性的可能措施,如能带改性和电子调制、空位工程、元素掺杂、非晶态工程调制等,以及影响NH3催化选择性的关键因素。如氢键效应和单原子/高度分散的位点等。此外,还分析了金属与金属/载体之间的相互作用以及约束工程、纳米工程等增强催化剂稳定性的策略。最后,本文总结了该技术在实践中面临的挑战,并展望了该技术在未来应用中的前景。
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引用次数: 0
Application of transition metal doped M-W18O49 in catalysis 过渡金属掺杂M-W18O49在催化中的应用
Q3 Energy Pub Date : 2025-10-01 DOI: 10.1016/S1872-5813(25)60550-0
Duojia REN , Wenxia SHI , Huixiang WANG , Jianghong WU , Wenting LÜ , Ping WANG , Baoliang LÜ
W18O49, a non-stoichiometric n-type semiconductor material with rich oxygen vacancies, exhibits excellent catalytic performance in optical, electrical, and thermal reactions. However, the inherent band structure of pristine W18O49 somewhat limits the enhancement of its catalytic activity. Transition metal ion doping emerges as an effective strategy to modify the internal atomic and electronic structures of this material. By incorporating transition metal atoms into the W18O49 lattice, it not only further increases the concentration of oxygen vacancies and introduces new active sites within W18O49, but also optimizes electron transport and band charge distribution, thereby enhancing its catalytic activity and broadening application scope in catalysis. This paper commences with an overview of the crystalline characteristics and band structure of W18O49, followed by an introduction to the synthesis method of this material. It then elaborates on the current modifications of W18O49 performance through transition metal doping and systematically discusses the typical applications of doped M-W18O49 in catalysis, including the reaction mechanisms involved in photocatalytic CO2 reduction, photocatalytic and electrocatalytic N2 fixation, electrocatalytic water splitting, and thermal catalytic oxidative desulfurization.
W18O49是一种富氧空位的非化学计量n型半导体材料,在光学、电学和热学反应中表现出优异的催化性能。然而,原始W18O49固有的能带结构在一定程度上限制了其催化活性的增强。过渡金属离子掺杂是改变这种材料内部原子和电子结构的有效策略。通过在W18O49晶格中加入过渡金属原子,不仅进一步增加了氧空位的浓度,在W18O49中引入了新的活性位点,而且优化了电子传递和带荷分布,从而提高了其催化活性,拓宽了在催化中的应用范围。本文首先概述了W18O49的晶体特性和能带结构,然后介绍了该材料的合成方法。然后阐述了目前通过过渡金属掺杂对W18O49性能的修饰,系统讨论了掺杂M-W18O49在催化中的典型应用,包括光催化CO2还原、光催化和电催化N2固定、电催化水裂解、热催化氧化脱硫等反应机理。
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引用次数: 0
Study on the synthesis of CeO2-Co3O4 catalyst by flame spray pyrolysis method and its catalytic oxidation performance for ethane 火焰喷雾热解法合成CeO2-Co3O4催化剂及其对乙烷的催化氧化性能研究
Q3 Energy Pub Date : 2025-10-01 DOI: 10.1016/S1872-5813(25)60548-2
Xianyan LÜ , Jiangliang HU , Jiancai HOU , Jiancheng WANG , Weiren BAO , Liping CHANG
The Ce5Co95 catalyst was synthesized using the method of flame spray pyrolysis (FSP) utilizing 2-ethylhexanoic acid (2-EHA) as an organic ligand. The effects on the catalytic oxidation performance of ethane caused by adding 2-EHA to the precursor solvent were systematically studied. The Ce5Co95-10%2-EHA catalyst exhibits excellent catalytic performance, with a t90 (temperature at which ethane conversion reaches 90%) of 293 °C at a weight hourly space velocity of 60000 mL/(g·h). The catalyst's physicochemical properties were characterized using XRD, BET, Raman, HRTEM, XPS, H2-TPR, O2-TPD and EPR techniques, which were effectively correlated with its catalytic performance. The introduction of 2-EHA significantly led to reduction in the catalyst's crystallite size, an increase in the specific surface area, and provision of additional active sites for the reaction. Additionally, it enhanced the Ce-Co interaction, resulting in the creation of abundant oxygen vacancies at the CeO2-Co3O4 interface. This phenomenon not only weakened the metal-oxygen bonds but also promoted the mobility of lattice oxygen, enhancing the catalyst's redox capability and optimizing its oxidation performance. The Ce5Co95-10%2-EHA catalyst also demonstrated outstanding thermal stability and reversible water tolerance. Moreover, the mechanism of ethane oxidation on the catalyst surface was investigated using in situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTS).
以2-乙基己酸(2-EHA)为有机配体,采用火焰喷雾热解法(FSP)合成Ce5Co95催化剂。系统地研究了在前驱溶剂中加入2-EHA对乙烷催化氧化性能的影响。Ce5Co95-10%2-EHA催化剂表现出优异的催化性能,在失重时空间速度为60000 mL/(g·h)时,t90(乙烷转化率达到90%的温度)为293℃。采用XRD、BET、Raman、HRTEM、XPS、H2-TPR、O2-TPD和EPR等技术对催化剂的理化性质进行了表征,并与催化剂的催化性能进行了有效关联。2-EHA的引入显著降低了催化剂的晶粒尺寸,增加了比表面积,并为反应提供了额外的活性位点。此外,它增强了Ce-Co相互作用,导致在CeO2-Co3O4界面上产生丰富的氧空位。这种现象不仅削弱了金属-氧键,而且促进了晶格氧的迁移性,增强了催化剂的氧化还原能力,优化了催化剂的氧化性能。Ce5Co95-10%2-EHA催化剂也表现出出色的热稳定性和可逆性耐水性。此外,利用原位漫反射红外傅立叶变换光谱(in situ DRIFTS)研究了乙烷在催化剂表面氧化的机理。
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引用次数: 0
Coal gasification fine slag and nitrogen-containing waste Co-hydrothermal preparation of porous materials for CO2 adsorption 煤气化细渣与含氮废渣共水热法制备吸附CO2的多孔材料
Q3 Energy Pub Date : 2025-10-01 DOI: 10.1016/S1872-5813(25)60560-3
Qingyun WANG , Xiaqing LIU , Li MA , Peng LÜ , Yonghui BAI
A new adsorbent was successfully prepared by hydrothermal treatment and chemical activation through coal gasification fine slag (CGFS) and blue algae (BA) as raw materials and used for CO2 capture. The CO2 chemisorption capacity of the adsorbent was further enhanced by taking advantage of the nitrogenous bases contained in the BA. In the hydrothermal process, the addition of BA significantly increased the content of pyrrole nitrogen in the adsorbent. In the activation process, pyrrole nitrogen gradually changed into pyridine nitrogen and graphite nitrogen. Increased BA addition result in a higher specific surface area and microporosity of the adsorbent. The CO2 adsorption performance test proved that the CGFS-50%-CA sample has the strongest CO2 adsorption capacity at low temperature, up to 15.59 cm3/g, which is mainly through physical adsorption, and the CGFS-10%-CA sample has the strongest CO2 adsorption capacity at high temperature, up to 7.31 cm3/g, which is mainly through chemical adsorption. CO2 uptake of the CGFS-10%-CA sample was well maintained after 10 cycles, with regeneration efficiencies above 99%. The results indicate that the novel adsorbents with coexistence of physical and chemical adsorption have great potential for CO2 adsorption applications.
以煤气化细渣(CGFS)和蓝藻(BA)为原料,采用水热法和化学活化法制备了一种新型吸附剂,并将其用于CO2捕集。利用BA中所含的氮基,进一步提高了吸附剂对CO2的化学吸附能力。在水热过程中,BA的加入显著提高了吸附剂中吡咯氮的含量。在活化过程中,吡咯氮逐渐转化为吡啶氮和石墨氮。BA添加量的增加导致吸附剂的比表面积和微孔率的增加。CO2吸附性能测试证明,CGFS-50%-CA样品在低温下CO2吸附能力最强,可达15.59 cm3/g,主要通过物理吸附;CGFS-10%-CA样品在高温下CO2吸附能力最强,可达7.31 cm3/g,主要通过化学吸附。经过10次循环后,CGFS-10%-CA样品的CO2吸收率保持良好,再生效率在99%以上。结果表明,这种物理吸附和化学吸附共存的新型吸附剂具有很大的CO2吸附应用潜力。
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引用次数: 0
Nickel-molybdenum alloy electrodeposited on nickel substrates for optimized hydrogen evolution reaction in acidic electrolytes 镍基电沉积镍钼合金,优化酸性电解液中析氢反应
Q3 Energy Pub Date : 2025-10-01 DOI: 10.1016/S1872-5813(25)60547-0
Haibo WANG , Zelin WU , Hui WEN , Zhiyong ZHAO , Chenbo WANG , Tongyu LU , Yuxuan GUO , Congwei WANG , Junying WANG
The utilization of nickel-based catalysts as alternatives to expensive platinum-based (Pt-based) materials for the hydrogen evolution reaction in acidic electrolytes has attracted considerable attention due to their potential for enabling cost-effective industrial applications. However, the unsatisfied cyclic stability and electrochemical activity limit their further application. In this work, nickel-molybdenum (Ni-Mo) alloy catalysts were successfully synthesized through a comprehensive process including electrodeposition, thermal annealing, and electrochemical activation. Owing to the synergistic interaction of molybdenum trinickelide (Ni3Mo) and molybdenum dioxide (MoO2) in Ni-Mo alloy, the catalyst display superior overall electrochemical properties. A low overpotential of 86 mV at 10 mA/cm2 and a Tafel slope of 74.0 mV/dec in 0.5 mol/L H2SO4 solution can be achieved. Notably, remarkable stability with negligible performance degradation even after 100 h could be maintained. This work presents a novel and effective strategy for the design and fabrication of high-performance, non-precious metal electrocatalysts for acidic water electrolysis.
利用镍基催化剂作为昂贵的铂基(pt基)材料在酸性电解质中进行析氢反应的替代品,由于其具有实现经济高效的工业应用的潜力,引起了相当大的关注。但循环稳定性和电化学活性的不理想限制了其进一步的应用。本文通过电沉积、热退火、电化学活化等综合工艺,成功合成了镍钼(Ni-Mo)合金催化剂。在Ni-Mo合金中,由于三氧化二钼(Ni3Mo)和二氧化钼(MoO2)的协同作用,该催化剂表现出优异的综合电化学性能。在0.5 mol/L H2SO4溶液中,可获得低过电位86 mV/ cm2和Tafel斜率74.0 mV/dec。值得注意的是,即使在100小时后,也可以保持显著的稳定性,性能下降可以忽略不计。本研究为设计和制造高性能、非贵金属的酸性电解电催化剂提供了一种新颖有效的策略。
{"title":"Nickel-molybdenum alloy electrodeposited on nickel substrates for optimized hydrogen evolution reaction in acidic electrolytes","authors":"Haibo WANG ,&nbsp;Zelin WU ,&nbsp;Hui WEN ,&nbsp;Zhiyong ZHAO ,&nbsp;Chenbo WANG ,&nbsp;Tongyu LU ,&nbsp;Yuxuan GUO ,&nbsp;Congwei WANG ,&nbsp;Junying WANG","doi":"10.1016/S1872-5813(25)60547-0","DOIUrl":"10.1016/S1872-5813(25)60547-0","url":null,"abstract":"<div><div>The utilization of nickel-based catalysts as alternatives to expensive platinum-based (Pt-based) materials for the hydrogen evolution reaction in acidic electrolytes has attracted considerable attention due to their potential for enabling cost-effective industrial applications. However, the unsatisfied cyclic stability and electrochemical activity limit their further application. In this work, nickel-molybdenum (Ni-Mo) alloy catalysts were successfully synthesized through a comprehensive process including electrodeposition, thermal annealing, and electrochemical activation. Owing to the synergistic interaction of molybdenum trinickelide (Ni<sub>3</sub>Mo) and molybdenum dioxide (MoO<sub>2</sub>) in Ni-Mo alloy, the catalyst display superior overall electrochemical properties. A low overpotential of 86 mV at 10 mA/cm<sup>2</sup> and a Tafel slope of 74.0 mV/dec in 0.5 mol/L H<sub>2</sub>SO<sub>4</sub> solution can be achieved. Notably, remarkable stability with negligible performance degradation even after 100 h could be maintained. This work presents a novel and effective strategy for the design and fabrication of high-performance, non-precious metal electrocatalysts for acidic water electrolysis.</div></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"53 10","pages":"Pages 1509-1518"},"PeriodicalIF":0.0,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145324628","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Research on the performance of photothermal catalytic CO2 hydrogenation to methanol using lanthanum- modified copper calcium titanate 镧改性钛酸铜钙光热催化CO2加氢制甲醇的性能研究
Q3 Energy Pub Date : 2025-09-01 DOI: 10.1016/S1872-5813(25)60563-9
LI jianyu , NA wei , GAO wengui , HE pengcheng
Perovskite oxide catalysts of copper calcium titanate with lanthanum (La) substituting for calcium sites were prepared by the sol-gel method, and their performance in the photothermal CO2 hydrogenation to methanol was experimentally investigated. Techniques such as XRD, SEM, CO2-TPD, H2-TPR, XPS, UV-Vis DRS, and EIS were employed to evaluate the advantages of La substitution for the copper calcium titanate catalysts. The results showed that after an appropriate amount of La substitution, the catalyst achieved a methanol space-time yield of 5.788 mmol/(g·h) under 0.8 MPa and 250 ℃ with illumination, which represents a significant improvement in catalytic performance compared to the unsubstituted catalyst. This enhancement is attributed to the promotion of oxygen vacancy formation by La substitution, which enhances the photothermal response efficiency of the catalyst and, consequently, its catalytic activity.
采用溶胶-凝胶法制备了镧取代钙位的钛酸铜钙钙钙氧化物催化剂,并对其在CO2光热加氢制甲醇中的性能进行了实验研究。采用XRD、SEM、CO2-TPD、H2-TPR、XPS、UV-Vis DRS、EIS等技术评价了钛酸铜钙催化剂取代La的优势。结果表明,在0.8 MPa、250℃光照条件下,适量的La取代后,催化剂的甲醇空时产率为5.788 mmol/(g·h),与未取代的催化剂相比,催化性能有显著提高。这种增强是由于La取代促进了氧空位的形成,从而提高了催化剂的光热响应效率,从而提高了催化活性。
{"title":"Research on the performance of photothermal catalytic CO2 hydrogenation to methanol using lanthanum- modified copper calcium titanate","authors":"LI jianyu ,&nbsp;NA wei ,&nbsp;GAO wengui ,&nbsp;HE pengcheng","doi":"10.1016/S1872-5813(25)60563-9","DOIUrl":"10.1016/S1872-5813(25)60563-9","url":null,"abstract":"<div><div>Perovskite oxide catalysts of copper calcium titanate with lanthanum (La) substituting for calcium sites were prepared by the sol-gel method, and their performance in the photothermal CO<sub>2</sub> hydrogenation to methanol was experimentally investigated. Techniques such as XRD, SEM, CO<sub>2</sub>-TPD, H<sub>2</sub>-TPR, XPS, UV-Vis DRS, and EIS were employed to evaluate the advantages of La substitution for the copper calcium titanate catalysts. The results showed that after an appropriate amount of La substitution, the catalyst achieved a methanol space-time yield of 5.788 mmol/(g·h) under 0.8 MPa and 250 ℃ with illumination, which represents a significant improvement in catalytic performance compared to the unsubstituted catalyst. This enhancement is attributed to the promotion of oxygen vacancy formation by La substitution, which enhances the photothermal response efficiency of the catalyst and, consequently, its catalytic activity.</div></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"53 9","pages":"Pages 1320-1329"},"PeriodicalIF":0.0,"publicationDate":"2025-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145108403","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Research progress on strategies to improve the carbon dioxide capture performance of MgO-based adsorbents 提高mgo基吸附剂二氧化碳捕集性能策略的研究进展
Q3 Energy Pub Date : 2025-09-01 DOI: 10.1016/S1872-5813(25)60545-7
ZHAO Yunrong , WANG Yaozu , NIU Yuqi , BIE Xuan , CHEN Rongjie , LI Qinghai , ZHANG Yanguo , ZHOU Hui
Carbon dioxide (CO2) emitted during the use of fossil fuels contributes to the global warming. Carbon capture, utilization and storage (CCUS) technology based on solid material adsorption is recognized as one of the most important means to effectively control and reduce the concentration of CO2. Magnesium oxide (MgO) is considered as an ideal adsorption material due to its high theoretical adsorption capacity, low regeneration energy consumption and wide temperature applicability. However, its actual adsorption capacity still needs to be further improved. Therefore, the internal reasons restricting the efficient adsorption of CO2 by MgO are introduced in this review. Meanwhile, the research progress on the preparation and modification of MgO based adsorbents in recent years is summarized. The preparation methods for enhancing the CO2 adsorption performance of MgO materials are reviewed, and the modification strategies of adsorbents are highlighted, for instance, microstructure modification of MgO, preparation of MgO composite adsorbents and molten salt doping modification. Furthermore, the mechanism behind different modification strategies is analyzed, moreover, the advantages and limitations of the above modification methods are summarized. Herein, the strategies to improve CO2 capture performance of MgO based adsorbents in recent years are reviewed and summarized. This review would provide insights for the design and preparation of new, cheap and efficient magnesium-based adsorbents in the future.
在使用化石燃料的过程中排放的二氧化碳(CO2)加剧了全球变暖。基于固体物质吸附的碳捕集、利用与封存(CCUS)技术是公认的有效控制和降低CO2浓度的重要手段之一。氧化镁(MgO)具有理论吸附容量大、再生能耗低、适用温度广等优点,被认为是一种理想的吸附材料。但其实际吸附能力仍需进一步提高。因此,本文介绍了制约MgO高效吸附CO2的内在原因。同时,综述了近年来MgO基吸附剂的制备和改性研究进展。综述了提高MgO材料CO2吸附性能的制备方法,重点介绍了吸附剂的改性策略,如MgO的微观结构改性、MgO复合吸附剂的制备和熔盐掺杂改性。分析了不同改性策略背后的机理,并总结了上述改性方法的优点和局限性。本文对近年来提高MgO基吸附剂CO2捕集性能的策略进行了综述和总结。为今后设计和制备新型、廉价、高效的镁基吸附剂提供参考。
{"title":"Research progress on strategies to improve the carbon dioxide capture performance of MgO-based adsorbents","authors":"ZHAO Yunrong ,&nbsp;WANG Yaozu ,&nbsp;NIU Yuqi ,&nbsp;BIE Xuan ,&nbsp;CHEN Rongjie ,&nbsp;LI Qinghai ,&nbsp;ZHANG Yanguo ,&nbsp;ZHOU Hui","doi":"10.1016/S1872-5813(25)60545-7","DOIUrl":"10.1016/S1872-5813(25)60545-7","url":null,"abstract":"<div><div>Carbon dioxide (CO<sub>2</sub>) emitted during the use of fossil fuels contributes to the global warming. Carbon capture, utilization and storage (CCUS) technology based on solid material adsorption is recognized as one of the most important means to effectively control and reduce the concentration of CO<sub>2</sub>. Magnesium oxide (MgO) is considered as an ideal adsorption material due to its high theoretical adsorption capacity, low regeneration energy consumption and wide temperature applicability. However, its actual adsorption capacity still needs to be further improved. Therefore, the internal reasons restricting the efficient adsorption of CO<sub>2</sub> by MgO are introduced in this review. Meanwhile, the research progress on the preparation and modification of MgO based adsorbents in recent years is summarized. The preparation methods for enhancing the CO<sub>2</sub> adsorption performance of MgO materials are reviewed, and the modification strategies of adsorbents are highlighted, for instance, microstructure modification of MgO, preparation of MgO composite adsorbents and molten salt doping modification. Furthermore, the mechanism behind different modification strategies is analyzed, moreover, the advantages and limitations of the above modification methods are summarized. Herein, the strategies to improve CO<sub>2</sub> capture performance of MgO based adsorbents in recent years are reviewed and summarized. This review would provide insights for the design and preparation of new, cheap and efficient magnesium-based adsorbents in the future.</div></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"53 9","pages":"Pages 1269-1282"},"PeriodicalIF":0.0,"publicationDate":"2025-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145108499","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Catalytic desorption performance of CO2-rich amine solution over SO2− 4/TiO2-HZSM-5 富co2胺溶液在SO2−4/TiO2-HZSM-5上的催化脱附性能
Q3 Energy Pub Date : 2025-09-01 DOI: 10.1016/S1872-5813(25)60559-7
SONG Wenqian , WEN Yuxin , KANG Guojun , LI Dekang , HU Haoquan , JIN Lijun , LU Shijian , YAN Zhong , LIU Pengfei
Amine-based solution absorption method, as the most mature CO2 capture technology, requires enhancing CO2 desorption performance while reducing energy consumption in desorption. A series of SO2− 4/TiO2-HZSM-5 catalysts with different TiO2 contents were prepared by sol-gel method using HZSM-5 as carrier and used in CO2 catalytic desorption of N-methyl-diethanolamine and piperazine blended amine solution. Results indicated that catalyst performance can be regulated by changing the loading amount of TiO2. When the mass ratio of TiO2 to HZSM-5 was 2/1, the resultant STH(2/1) catalyst had large mesoporous surface area and abundant acidic sites and exhibited excellent catalytic performance. Compared with non-catalytic system, CO2 desorption amount of the entire desorption increased by 15.38% and relative heat duty decreased by 21.69%. Meanwhile, STH(2/1) exhibited good activity and stability after regeneration cycles and had no impact on CO2 absorption performance. Larger mesoporous surface area of catalyst facilitated sufficient contact between reactants and acidic sites. Abundant amount of strong acid sites and Brønsted acid sites provided a large amount of H+, promoting the decomposition of carbamate and deprotonation of protonated amines. The combined action of mesoporous surface area, strong acid sites and Brønsted acid sites promoted CO2 desorption. In addition, a possible mechanism for CO2 desorption catalyzed by SO2− 4/TiO2-HZSM-5 was proposed.
胺基溶液吸收法作为最成熟的CO2捕集技术,要求在提高CO2解吸性能的同时降低解吸过程中的能耗。以HZSM-5为载体,采用溶胶-凝胶法制备了一系列不同TiO2含量的SO2−4/TiO2-HZSM-5催化剂,用于n -甲基-二乙醇胺和哌嗪混合胺溶液的CO2催化解吸。结果表明,通过改变TiO2的负载量可以调节催化剂的性能。当TiO2与HZSM-5的质量比为2/1时,得到的STH(2/1)催化剂具有较大的介孔表面积和丰富的酸性位点,具有优异的催化性能。与非催化体系相比,整个脱附过程的CO2脱附量提高了15.38%,相对热负荷降低了21.69%。同时,STH(2/1)在再生循环后表现出良好的活性和稳定性,对CO2的吸收性能没有影响。催化剂的介孔表面积较大,有利于反应物与酸性位点之间的充分接触。大量的强酸位点和Brønsted酸位点提供了大量的H+,促进氨基甲酸酯的分解和质子化胺的去质子化。介孔表面积、强酸位和Brønsted酸位的共同作用促进了CO2的脱附。此外,提出了SO2−4/TiO2-HZSM-5催化CO2脱附的可能机理。
{"title":"Catalytic desorption performance of CO2-rich amine solution over SO2− 4/TiO2-HZSM-5","authors":"SONG Wenqian ,&nbsp;WEN Yuxin ,&nbsp;KANG Guojun ,&nbsp;LI Dekang ,&nbsp;HU Haoquan ,&nbsp;JIN Lijun ,&nbsp;LU Shijian ,&nbsp;YAN Zhong ,&nbsp;LIU Pengfei","doi":"10.1016/S1872-5813(25)60559-7","DOIUrl":"10.1016/S1872-5813(25)60559-7","url":null,"abstract":"<div><div>Amine-based solution absorption method, as the most mature CO<sub>2</sub> capture technology, requires enhancing CO<sub>2</sub> desorption performance while reducing energy consumption in desorption. A series of SO2− 4/TiO<sub>2</sub>-HZSM-5 catalysts with different TiO<sub>2</sub> contents were prepared by sol-gel method using HZSM-5 as carrier and used in CO<sub>2</sub> catalytic desorption of <em>N</em>-methyl-diethanolamine and piperazine blended amine solution. Results indicated that catalyst performance can be regulated by changing the loading amount of TiO<sub>2</sub>. When the mass ratio of TiO<sub>2</sub> to HZSM-5 was 2/1, the resultant STH(2/1) catalyst had large mesoporous surface area and abundant acidic sites and exhibited excellent catalytic performance. Compared with non-catalytic system, CO<sub>2</sub> desorption amount of the entire desorption increased by 15.38% and relative heat duty decreased by 21.69%. Meanwhile, STH(2/1) exhibited good activity and stability after regeneration cycles and had no impact on CO<sub>2</sub> absorption performance. Larger mesoporous surface area of catalyst facilitated sufficient contact between reactants and acidic sites. Abundant amount of strong acid sites and Brønsted acid sites provided a large amount of H<sup>+</sup>, promoting the decomposition of carbamate and deprotonation of protonated amines. The combined action of mesoporous surface area, strong acid sites and Brønsted acid sites promoted CO<sub>2</sub> desorption. In addition, a possible mechanism for CO<sub>2</sub> desorption catalyzed by SO2− 4/TiO<sub>2</sub>-HZSM-5 was proposed.</div></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"53 9","pages":"Pages 1342-1353"},"PeriodicalIF":0.0,"publicationDate":"2025-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145108398","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
The effect of non-free calcium on dissolution-polymerization reaction mechanism of coal gasification slag 非游离钙对煤气化渣溶聚反应机理的影响
Q3 Energy Pub Date : 2025-09-01 DOI: 10.1016/S1872-5813(25)60566-4
WANG Ji , MA Xu , GUO Hanghao , WANG Huixia , QU Yongping , JIAO Weizhou , MA Zhibin
Coal gasification slag is an excellent raw material for preparation of cementitious materials. Due to the addition of calcium-based additives, the content of non-free calcium in silicon/aluminum-rich coal gasification slag is relatively high. Thus, the influence of non-free calcium on leaching of elemental and formation mechanisms of cementitious phase were investigated by this paper. The results indicate that non-free calcium primarily disrupts the Al−O−Al bridges in the aluminosilicate glass phase, leading to decreased polymerization degree of slag. The compressive strength of cementitious materials is affected by alkali activation concentration and polymerization degree of slag. Under low-alkali conditions, as the calcium content in the gasification slag increases, the compressive strength of the cementitious material increases firstly and then decreases. Increased calcium promotes leaching of Al, however, large amounts of dissolved calcium tend to form cementitious phases and Ca(OH)2, which can hinder leaching of ions and formation of gel. In high-alkali environments, non-free calcium enhances the compressive strength of cementitious material. Glass phase in slag was destroyed by OH⁻, and leaching rates of Si and Al in slag with high-calcium increase, which lead to more C-A-S-H in cementitious material. Additionally, elevated alkalinity promotes the crystallization of sodium-minerals such as zeolites and sodalite.
煤气化渣是制备胶凝材料的优良原料。由于添加了钙基添加剂,富硅/富铝煤气化渣中的非游离钙含量较高。因此,本文研究了非游离钙对元素浸出的影响及胶凝相的形成机制。结果表明:非游离钙主要破坏铝硅酸盐玻璃相中的Al - O - Al桥,导致熔渣聚合度降低;胶凝材料的抗压强度受碱活化浓度和矿渣聚合程度的影响。低碱条件下,随着气化渣中钙含量的增加,胶凝材料的抗压强度先增大后减小。增加的钙促进Al的浸出,但大量溶解的钙容易形成胶凝相和Ca(OH)2,阻碍离子的浸出和凝胶的形成。在高碱环境下,非游离钙提高了胶凝材料的抗压强度。OH - 9破坏了渣中的玻璃相,高钙渣中Si和Al的浸出率增加,导致胶凝材料中C-A-S-H含量增加。此外,碱度的升高促进了沸石和钠石等钠矿物的结晶。
{"title":"The effect of non-free calcium on dissolution-polymerization reaction mechanism of coal gasification slag","authors":"WANG Ji ,&nbsp;MA Xu ,&nbsp;GUO Hanghao ,&nbsp;WANG Huixia ,&nbsp;QU Yongping ,&nbsp;JIAO Weizhou ,&nbsp;MA Zhibin","doi":"10.1016/S1872-5813(25)60566-4","DOIUrl":"10.1016/S1872-5813(25)60566-4","url":null,"abstract":"<div><div>Coal gasification slag is an excellent raw material for preparation of cementitious materials. Due to the addition of calcium-based additives, the content of non-free calcium in silicon/aluminum-rich coal gasification slag is relatively high. Thus, the influence of non-free calcium on leaching of elemental and formation mechanisms of cementitious phase were investigated by this paper. The results indicate that non-free calcium primarily disrupts the Al−O−Al bridges in the aluminosilicate glass phase, leading to decreased polymerization degree of slag. The compressive strength of cementitious materials is affected by alkali activation concentration and polymerization degree of slag. Under low-alkali conditions, as the calcium content in the gasification slag increases, the compressive strength of the cementitious material increases firstly and then decreases. Increased calcium promotes leaching of Al, however, large amounts of dissolved calcium tend to form cementitious phases and Ca(OH)<sub>2</sub>, which can hinder leaching of ions and formation of gel. In high-alkali environments, non-free calcium enhances the compressive strength of cementitious material. Glass phase in slag was destroyed by OH⁻, and leaching rates of Si and Al in slag with high-calcium increase, which lead to more C-A-S-H in cementitious material. Additionally, elevated alkalinity promotes the crystallization of sodium-minerals such as zeolites and sodalite.</div></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"53 9","pages":"Pages 1416-1426"},"PeriodicalIF":0.0,"publicationDate":"2025-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145108399","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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