Pub Date : 2024-12-25DOI: 10.1016/j.mtcata.2024.100087
Huamei Li , Mengyuan Li , Lingling Liao , Han Yang , Kun Xiang , Guoqiang Luo , Mingjiang Xie
The challenge of the complex oxygen evolution reaction (OER) currently impedes the efficient production of hydrogen via electrolytic water splitting. To address this issue, the development and improvement of effective electrocatalysts are required. LiCoO2, a key material in lithium-ion batteries, has shown promising potential as an electrocatalyst for electrochemical energy conversion. However, OER catalysts derived from LiCoO2 have faced obstacles such as high overpotential and a complicated preparation process. In this study, the preparation method is adjusted to optimize the synthesis of Li1-xCoO2 with a defective structure, resulting in an impressive overpotential of only 290 mV at a current density of 100 mA cm−2 and a remarkable Tafel slope of 15.2 mV dec−1. The exceptional catalytic activity of Li1-xCoO2 can be attributed to the absence of Li, which triggers oxidative alterations in the electronic structure of Co. Density functional theory (DFT) calculations reveal that Li defects can influence the d-band center of active Co sites, enhancing the adsorption capabilities of Co sites towards *OOH intermediates and increasing the conductivity of the electrocatalyst during the OER process. These alterations improve the velocity of the crucial step in the reaction, ultimately boosting the catalyst's overall performance and efficiency.
复杂析氧反应（OER）的挑战目前阻碍了通过电解水分解高效生产氢。为了解决这一问题，需要开发和改进有效的电催化剂。LiCoO2是锂离子电池的关键材料，作为电化学能量转换的电催化剂，具有广阔的应用前景。然而，LiCoO2衍生的OER催化剂面临着高过电位和复杂的制备工艺等障碍。在本研究中，通过调整制备方法，优化合成了具有缺陷结构的Li1-xCoO2，在电流密度为100 mA cm−2时，过电位仅为290 mV， Tafel斜率为15.2 mV dec−1。Li1-xCoO2的特殊催化活性可归因于Li的缺失，这引发了Co电子结构的氧化改变。密度泛函理论（DFT）计算表明，Li缺陷可以影响活性Co位的d带中心，增强Co位对*OOH中间体的吸附能力，并在OER过程中提高电催化剂的导电性。这些改变提高了反应中关键步骤的速度，最终提高了催化剂的整体性能和效率。
{"title":"Boosting oxygen evolution of LiCoO2 electrocatalysts via lithium defect","authors":"Huamei Li , Mengyuan Li , Lingling Liao , Han Yang , Kun Xiang , Guoqiang Luo , Mingjiang Xie","doi":"10.1016/j.mtcata.2024.100087","DOIUrl":"10.1016/j.mtcata.2024.100087","url":null,"abstract":"<div><div>The challenge of the complex oxygen evolution reaction (OER) currently impedes the efficient production of hydrogen via electrolytic water splitting. To address this issue, the development and improvement of effective electrocatalysts are required. LiCoO<sub>2</sub>, a key material in lithium-ion batteries, has shown promising potential as an electrocatalyst for electrochemical energy conversion. However, OER catalysts derived from LiCoO<sub>2</sub> have faced obstacles such as high overpotential and a complicated preparation process. In this study, the preparation method is adjusted to optimize the synthesis of Li<sub>1-x</sub>CoO<sub>2</sub> with a defective structure, resulting in an impressive overpotential of only 290 mV at a current density of 100 mA cm<sup>−2</sup> and a remarkable Tafel slope of 15.2 mV dec<sup>−1</sup>. The exceptional catalytic activity of Li<sub>1-x</sub>CoO<sub>2</sub> can be attributed to the absence of Li, which triggers oxidative alterations in the electronic structure of Co. Density functional theory (DFT) calculations reveal that Li defects can influence the d-band center of active Co sites, enhancing the adsorption capabilities of Co sites towards *OOH intermediates and increasing the conductivity of the electrocatalyst during the OER process. These alterations improve the velocity of the crucial step in the reaction, ultimately boosting the catalyst's overall performance and efficiency.</div></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"8 ","pages":"Article 100087"},"PeriodicalIF":0.0,"publicationDate":"2024-12-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143148539","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-12-10DOI: 10.1016/j.mtcata.2024.100081
Jian Chen , Yixin Huang , Liu Wan, Cheng Du, Yan Zhang, Mingjiang Xie
The development of CdS-based photocatalysts with the appropriate bandgap structure, impressive optical response, and long-lasting reusability is both crucial and challenging. The heterogeneous catalyst, made up of polytriazine and CdS, demonstrates exceptional photogenerated charge separation and transfer capabilities, as well as superior CO2 adsorption abilities. In this study, we have shown that the CO2 photoassisted reduction efficiency of CdS nanosheets can be significantly improved through surface modification with a polytriazine polymer coating. The PP@CdS photocatalyst has been thoroughly characterized using techniques such as XRD, TEM, SEM, N2 adsorption-desorption, CO2 adsorption, DRS, XPS, and photoelectric performance tests. The catalytic performance of the PP@CdS was assessed through photoassisted CO2 reduction reactions under visible light irradiation in an aqueous medium at 25 ℃. Owing to its enhanced CO2 adsorption capacity and the efficient separation and utilization of photogenerated electrons, the PP@CdS photocatalyst demonstrated a CO yield (6.7 μmol/g/h) 1.3 times greater and a CH4 yield (4.2 μmol/g/h) 1.3 times higher than that of bare CdS nanosheets. Furthermore, the PP@CdS photocatalyst demonstrated outstanding reusability in CO2 reduction reactions. This study presents a novel approach to enhancing the CO2 adsorption capacity and modulating the bandgap structure of polymer-coated semiconductor materials.
{"title":"Polytriazine@CdS nanosheets as photosensitizer free catalyst for efficient photocatalytic reduction of CO2","authors":"Jian Chen , Yixin Huang , Liu Wan, Cheng Du, Yan Zhang, Mingjiang Xie","doi":"10.1016/j.mtcata.2024.100081","DOIUrl":"10.1016/j.mtcata.2024.100081","url":null,"abstract":"<div><div>The development of CdS-based photocatalysts with the appropriate bandgap structure, impressive optical response, and long-lasting reusability is both crucial and challenging. The heterogeneous catalyst, made up of polytriazine and CdS, demonstrates exceptional photogenerated charge separation and transfer capabilities, as well as superior CO<sub>2</sub> adsorption abilities. In this study, we have shown that the CO<sub>2</sub> photoassisted reduction efficiency of CdS nanosheets can be significantly improved through surface modification with a polytriazine polymer coating. The PP@CdS photocatalyst has been thoroughly characterized using techniques such as XRD, TEM, SEM, N<sub>2</sub> adsorption-desorption, CO<sub>2</sub> adsorption, DRS, XPS, and photoelectric performance tests. The catalytic performance of the PP@CdS was assessed through photoassisted CO<sub>2</sub> reduction reactions under visible light irradiation in an aqueous medium at 25 ℃. Owing to its enhanced CO<sub>2</sub> adsorption capacity and the efficient separation and utilization of photogenerated electrons, the PP@CdS photocatalyst demonstrated a CO yield (6.7 μmol/g/h) 1.3 times greater and a CH<sub>4</sub> yield (4.2 μmol/g/h) 1.3 times higher than that of bare CdS nanosheets. Furthermore, the PP@CdS photocatalyst demonstrated outstanding reusability in CO<sub>2</sub> reduction reactions. This study presents a novel approach to enhancing the CO<sub>2</sub> adsorption capacity and modulating the bandgap structure of polymer-coated semiconductor materials.</div></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"8 ","pages":"Article 100081"},"PeriodicalIF":0.0,"publicationDate":"2024-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143148540","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-12-01DOI: 10.1016/j.mtcata.2024.100076
Ángel Morales-García , José D. Gouveia , Anna Vidal López , Aleix Comas-Vives , Francesc Viñes , José R.B. Gomes , Francesc Illas
Pristine Mo2C MXene has been recently highlighted as a highly active and robust catalyst for the reverse water gas shift (RWGS) reaction. Here, first-principles calculations based on density functional theory (DFT) coupled with mean-field microkinetic (MKM) simulations are performed to investigate the effects of the atomic layer stacking and the surface functionalization with oxo groups on the catalyst performance. The calculated data show that ABA stacked MXene has a reactivity higher than the corresponding ABC counterpart. Moreover, a 2/3 surface monolayer oxygen coverage on both stackings (i.e., Mo2CO4/3 MXene) enhances the overall reactivity compared with their pristine Mo2C counterparts. The reactivity enhancement is small for the more stable ABA-stacked model, with a CO gas production aligned with experimental reports. However, the partial O-surface termination in the MXene with ABC stacking offers a more enhanced reactivity, supported by the higher CO gas production for the Mo2C MXene models here considered. Thus, the MXene stacking and its functionalization are key aspects affecting the performance of the Mo2C MXene for the RGWS reaction, which must be considered for realistic catalytic applications of MXenes.
{"title":"MXene termination and stacking bias on the reverse water gas shift reaction catalysis","authors":"Ángel Morales-García , José D. Gouveia , Anna Vidal López , Aleix Comas-Vives , Francesc Viñes , José R.B. Gomes , Francesc Illas","doi":"10.1016/j.mtcata.2024.100076","DOIUrl":"10.1016/j.mtcata.2024.100076","url":null,"abstract":"<div><div>Pristine Mo<sub>2</sub>C MXene has been recently highlighted as a highly active and robust catalyst for the reverse water gas shift (RWGS) reaction. Here, first-principles calculations based on density functional theory (DFT) coupled with mean-field microkinetic (MKM) simulations are performed to investigate the effects of the atomic layer stacking and the surface functionalization with oxo groups on the catalyst performance. The calculated data show that ABA stacked MXene has a reactivity higher than the corresponding ABC counterpart. Moreover, a <sup>2</sup>/<sub>3</sub> surface monolayer oxygen coverage on both stackings (<em>i.e.</em>, Mo<sub>2</sub>CO<sub>4/3</sub> MXene) enhances the overall reactivity compared with their pristine Mo<sub>2</sub>C counterparts. The reactivity enhancement is small for the more stable ABA-stacked model, with a CO gas production aligned with experimental reports. However, the partial O-surface termination in the MXene with ABC stacking offers a more enhanced reactivity, supported by the higher CO gas production for the Mo<sub>2</sub>C MXene models here considered. Thus, the MXene stacking and its functionalization are key aspects affecting the performance of the Mo<sub>2</sub>C MXene for the RGWS reaction, which must be considered for realistic catalytic applications of MXenes.</div></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"7 ","pages":"Article 100076"},"PeriodicalIF":0.0,"publicationDate":"2024-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142746005","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-12-01DOI: 10.1016/j.mtcata.2024.100079
Meiling Liu , Cuili Xiang , Yongjin Zou , Fen Xu , Lixian Sun , Ningbo Qin
The performance of single-component hydrogen evolution reaction (HER) electrocatalysts in terms of physicochemical properties and electrocatalytic efficiency has shown limitations for large-scale industrial applications. Consequently, developing new HER electrocatalysts with superior performance and mature technology is crucial for advancing this field. In this study, nickel foam/reduced graphene oxide/CoNi2S4-MoO2 (NF/rGO/CoNi2S4-MoO2) was prepared using a combination of water bath and two-step hydrothermal methods. Reduced graphene oxide (rGO) enhances the catalyst’s conductivity and induces uniform distribution of CoNi2S4. The sheet-like CoNi2S4 provides numerous active sites for the vertically distributed MoO2 nanosheets, reducing agglomeration and ensuring even distribution on the surface. The synergistic effect among rGO, CoNi2S4, and MoO2, along with their unique structures, facilitates charge transfer, enhancing the material’s electrochemical hydrogen evolution capabilities even more. The synthesized NF/rGO/CoNi2S4-MoO2 nanosheets exhibited excellent electrocatalytic performance. The overpotential of NF/rGO/CoNi2S4-MoO2 was as low as 65 mV in a 1.0 M KOH solution at a current density of 10 mA·cm−2, and the Tafel slope was 96.48 mV·dec−1.
{"title":"Nickel foam/reduced graphene oxide/CoNi2S4-MoO2 nanosheets with a core–shell structure formed: An efficient electrocatalyst for the hydrogen evolution reaction","authors":"Meiling Liu , Cuili Xiang , Yongjin Zou , Fen Xu , Lixian Sun , Ningbo Qin","doi":"10.1016/j.mtcata.2024.100079","DOIUrl":"10.1016/j.mtcata.2024.100079","url":null,"abstract":"<div><div>The performance of single-component hydrogen evolution reaction (HER) electrocatalysts in terms of physicochemical properties and electrocatalytic efficiency has shown limitations for large-scale industrial applications. Consequently, developing new HER electrocatalysts with superior performance and mature technology is crucial for advancing this field. In this study, nickel foam/reduced graphene oxide/CoNi<sub>2</sub>S<sub>4</sub>-MoO<sub>2</sub> (NF/rGO/CoNi<sub>2</sub>S<sub>4</sub>-MoO<sub>2</sub>) was prepared using a combination of water bath and two-step hydrothermal methods. Reduced graphene oxide (rGO) enhances the catalyst’s conductivity and induces uniform distribution of CoNi<sub>2</sub>S<sub>4</sub>. The sheet-like CoNi<sub>2</sub>S<sub>4</sub> provides numerous active sites for the vertically distributed MoO<sub>2</sub> nanosheets, reducing agglomeration and ensuring even distribution on the surface. The synergistic effect among rGO, CoNi<sub>2</sub>S<sub>4</sub>, and MoO<sub>2</sub>, along with their unique structures, facilitates charge transfer, enhancing the material’s electrochemical hydrogen evolution capabilities even more. The synthesized NF/rGO/CoNi<sub>2</sub>S<sub>4</sub>-MoO<sub>2</sub> nanosheets exhibited excellent electrocatalytic performance. The overpotential of NF/rGO/CoNi<sub>2</sub>S<sub>4</sub>-MoO<sub>2</sub> was as low as 65 mV in a 1.0 M KOH solution at a current density of 10 mA·cm<sup>−2</sup>, and the Tafel slope was 96.48 mV·dec<sup>−1</sup>.</div></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"7 ","pages":"Article 100079"},"PeriodicalIF":0.0,"publicationDate":"2024-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143137083","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Understanding the behavior of noble-metal catalysts is a key point of catalysis research aimed at reducing the environmental and economic costs associated with the increased use of automobiles. In this study, the atomic-behaviors of Ru and Pd atoms in PdRu solid-solution nanoparticles (NPs) supported on CeO2-ZrO2 (CZ) as a Rh-free three-way catalyst in a modeled three-way catalytic reaction (TWCR) were elucidated using a gas conversion analysis, transmission electron microscopy, and in-situ X-ray absorption fine structure spectroscopy. We found that the PdRu NPs enlarged by the annealing effect separated a smaller grain size with the Pd-rich and Ru-rich phase under TWCR. Most of the oxidation and reduction reactions under the modeled TWCR occurred on the Ru. However, the Pd metals acted as a major role of the reduction of NO gas and oxidation of CO and C3H6 gas. Ru atoms just is a minor role during the modeled TWCR. This study demonstrates the potential of PdRu NPs as a three-way catalyst and reveals the atomic-behavior and catalytic role under the modeled TWCR.
{"title":"Atomic behaviors in PdRu solid-solution nanoparticles on CeO2-ZrO2 support for the three-way catalytic reaction","authors":"Okkyun Seo , Akhil Tayal , Jaemyung Kim , Kohei Kusada , Tomokazu Yamamoto , Jiayi Tang , Satoshi Hiroi , Chulho Song , Katsutoshi Sato , Katsutoshi Nagaoka , Masaaki Haneda , Kazuo Kato , Syo Matsumura , Hiroshi Kitagawa , Osami Sakata","doi":"10.1016/j.mtcata.2024.100078","DOIUrl":"10.1016/j.mtcata.2024.100078","url":null,"abstract":"<div><div>Understanding the behavior of noble-metal catalysts is a key point of catalysis research aimed at reducing the environmental and economic costs associated with the increased use of automobiles. In this study, the atomic-behaviors of Ru and Pd atoms in PdRu solid-solution nanoparticles (NPs) supported on CeO<sub>2</sub>-ZrO<sub>2</sub> (CZ) as a Rh-free three-way catalyst in a modeled three-way catalytic reaction (TWCR) were elucidated using a gas conversion analysis, transmission electron microscopy, and <em>in</em>-<em>situ</em> X-ray absorption fine structure spectroscopy. We found that the PdRu NPs enlarged by the annealing effect separated a smaller grain size with the Pd-rich and Ru-rich phase under TWCR. Most of the oxidation and reduction reactions under the modeled TWCR occurred on the Ru. However, the Pd metals acted as a major role of the reduction of NO gas and oxidation of CO and C<sub>3</sub>H<sub>6</sub> gas. Ru atoms just is a minor role during the modeled TWCR. This study demonstrates the potential of PdRu NPs as a three-way catalyst and reveals the atomic-behavior and catalytic role under the modeled TWCR.</div></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"7 ","pages":"Article 100078"},"PeriodicalIF":0.0,"publicationDate":"2024-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142746480","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The purpose of this study is to develop a visible light responsive photocatalyst that can remove such environmental pollutants as polysulfide anions and simultaneously generate clean hydrogen energy. An environmentally friendly copper indium sulfide (CuInS2, CIS) nano-colloid was synthesized in aqueous medium for the design of such a photocatalyst. Characterization of the hydrophilic CIS with different In/Cu ratios were studied by XRD, Raman, UV-Vis, photoluminescence spectroscopy. These results showed that the long-lived photoexcited electrons in the CIS with higher In/Cu ratio can be expected to achieve efficient interaction with the reactant molecules. On the photocatalytic activity of CIS, the effect of such various supports as TiO2, and In/Cu ratio of CIS on the reaction promotion was examined. The CIS deposited TiO2 (CIS-TiO2) showed higher photocatalytic activity than bulk CIS, and the indium sulfide-richer CIS-TiO2 showed better performance. The indium sulfide moiety participates in the compensation of the defect sites in the CIS as well as the interaction between In-rich CIS and TiO2 can achieve effective charge carrier separation. This is the first report finding that the indium-richer CuInS2 plays an important role in an improvement of the photocatalytic activity.
{"title":"Effect of the indium sulfide phase in CuInS2-TiO2 photocatalysts to boost hydrogen evolution by water splitting","authors":"Mizuki Inada , Shizuki Yase , Atsune Tada , Takuma Yamane , Yuki Miyaji , Masanari Hirahara , Yoshiyuki Harada , Syuji Fujii , Takashi Fukushima , Satoru Dohshi , Shinya Higashimoto","doi":"10.1016/j.mtcata.2024.100080","DOIUrl":"10.1016/j.mtcata.2024.100080","url":null,"abstract":"<div><div>The purpose of this study is to develop a visible light responsive photocatalyst that can remove such environmental pollutants as polysulfide anions and simultaneously generate clean hydrogen energy. An environmentally friendly copper indium sulfide (CuInS<sub>2</sub>, CIS) nano-colloid was synthesized in aqueous medium for the design of such a photocatalyst. Characterization of the hydrophilic CIS with different In/Cu ratios were studied by XRD, Raman, UV-Vis, photoluminescence spectroscopy. These results showed that the long-lived photoexcited electrons in the CIS with higher In/Cu ratio can be expected to achieve efficient interaction with the reactant molecules. On the photocatalytic activity of CIS, the effect of such various supports as TiO<sub>2</sub>, and In/Cu ratio of CIS on the reaction promotion was examined. The CIS deposited TiO<sub>2</sub> (CIS-TiO<sub>2</sub>) showed higher photocatalytic activity than bulk CIS, and the indium sulfide-richer CIS-TiO<sub>2</sub> showed better performance. The indium sulfide moiety participates in the compensation of the defect sites in the CIS as well as the interaction between In-rich CIS and TiO<sub>2</sub> can achieve effective charge carrier separation. This is the first report finding that the indium-richer CuInS<sub>2</sub> plays an important role in an improvement of the photocatalytic activity.</div></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"7 ","pages":"Article 100080"},"PeriodicalIF":0.0,"publicationDate":"2024-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143137084","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-26DOI: 10.1016/j.mtcata.2024.100077
Arsh Ismaili, Gurwinder Singh, CI Sathish, Kavitha Ramadass, Vinay Naral, Stalin Joseph, Mercy Benzigar, Muhammad Ibrar Ahmed, Ajayan Vinu
Mesoporous materials are flourishing across every major research discipline, including carbon capture and conversion, energy storage, biomedical, photocatalysis, optics, and magnetics, and their promising potential has led to a flurry of publications. Among these applications, CO2 conversion using porous heterogeneous catalysts such as zeolites, clays, and mesoporous materials gained much attention in recent years as it has the potential to offer a solution for global warming. Although various porous catalysts have been used for CO2 conversion, mesoporous materials are particularly interesting owing to their large specific surface area, pore volume and pore diameter. These properties can be effectively utilized for creating unique catalytically active sites by loading metal or metal oxide species with high dispersion which are highly critical for efficient CO2 conversion. There have also been a significant number of reports on the direct use of mesoporous metal oxides, sulfides and/or phosphides, which exhibit appealing results for CO2 conversion as these inherently contain metal sites, and mesoporosity addition to them is an added advantage. Their continuous evolution warrants more sophisticated research to unveil their hidden properties by engaging in highly advanced characterization. The major emphasis of this review is to discuss various types of mesoporous materials mentioned above and their functionalized derivatives for CO2 conversion to mainly C1 products. The diverse range of mesoporous materials covered in this review will provide the readers with the opportunity to delve into their specific properties that control the efficiency of CO2 conversion.
介孔材料在碳捕获与转化、能量存储、生物医学、光催化、光学和磁学等各个主要研究学科中都得到了蓬勃发展，其巨大潜力已引发大量论文发表。在这些应用中，使用多孔异质催化剂（如沸石、粘土和介孔材料）进行二氧化碳转化近年来备受关注，因为它有可能为全球变暖提供解决方案。虽然各种多孔催化剂已被用于二氧化碳转化，但介孔材料因其较大的比表面积、孔体积和孔直径而尤其引人关注。可以有效利用这些特性，通过装载高分散度的金属或金属氧化物来创建独特的催化活性位点，这对于高效的二氧化碳转化非常关键。此外，还有大量关于直接使用介孔金属氧化物、硫化物和/或磷化物的报道，由于这些物质本身含有金属位点，因此在二氧化碳转化方面表现出令人满意的效果，而添加介孔也是一个额外的优势。它们的不断发展需要进行更复杂的研究，通过高度先进的表征揭示其隐藏的特性。本综述的主要重点是讨论上述各种类型的介孔材料及其功能化衍生物，用于将 CO2 转化为主要是 C1 产物。本综述中涉及的各种介孔材料将为读者提供机会，深入探讨它们控制二氧化碳转化效率的具体特性。
{"title":"Recent developments in functionalized mesoporous materials for CO2 conversion","authors":"Arsh Ismaili, Gurwinder Singh, CI Sathish, Kavitha Ramadass, Vinay Naral, Stalin Joseph, Mercy Benzigar, Muhammad Ibrar Ahmed, Ajayan Vinu","doi":"10.1016/j.mtcata.2024.100077","DOIUrl":"10.1016/j.mtcata.2024.100077","url":null,"abstract":"<div><div>Mesoporous materials are flourishing across every major research discipline, including carbon capture and conversion, energy storage, biomedical, photocatalysis, optics, and magnetics, and their promising potential has led to a flurry of publications. Among these applications, CO<sub>2</sub> conversion using porous heterogeneous catalysts such as zeolites, clays, and mesoporous materials gained much attention in recent years as it has the potential to offer a solution for global warming. Although various porous catalysts have been used for CO<sub>2</sub> conversion, mesoporous materials are particularly interesting owing to their large specific surface area, pore volume and pore diameter. These properties can be effectively utilized for creating unique catalytically active sites by loading metal or metal oxide species with high dispersion which are highly critical for efficient CO<sub>2</sub> conversion. There have also been a significant number of reports on the direct use of mesoporous metal oxides, sulfides and/or phosphides, which exhibit appealing results for CO<sub>2</sub> conversion as these inherently contain metal sites, and mesoporosity addition to them is an added advantage. Their continuous evolution warrants more sophisticated research to unveil their hidden properties by engaging in highly advanced characterization. The major emphasis of this review is to discuss various types of mesoporous materials mentioned above and their functionalized derivatives for CO<sub>2</sub> conversion to mainly C1 products. The diverse range of mesoporous materials covered in this review will provide the readers with the opportunity to delve into their specific properties that control the efficiency of CO<sub>2</sub> conversion.</div></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"7 ","pages":"Article 100077"},"PeriodicalIF":0.0,"publicationDate":"2024-11-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142724113","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-07DOI: 10.1016/j.mtcata.2024.100075
Julio C. Fernandes P. Brito , Geo Paul , Claudio Cassino , Ivana Miletto , Leonardo Marchese , Enrica Gianotti
Bi-functional catalysts possess various catalytic sites and can catalyze different types of reactions in a single-pot cascade manner. Herein, we report the synthesis and characterization of mono- and bifunctional silica-based mesoporous hybrid catalysts involving acid and base active sites. The ability for cooperative catalysis has been investigated using a multi-technique approach involving powder X-ray diffraction, FT-IR, and multinuclear MAS NMR spectroscopy, as well as thermogravimetric analysis. To elucidate the nature and strength of multifunctional catalytic sites, different types of probe molecules were employed and studied using spectroscopic techniques. The results show that the activity of the mesoporous surface-grafted acid and/or base sites is directly related to the intimacy criterion, the separation between the different types of catalytic sites. The presence or absence of mutual interactions between the different catalytic sites dictates the selectivity and yield of the reactions.
双功能催化剂具有不同的催化位点，能以单锅级联方式催化不同类型的反应。在此，我们报告了涉及酸和碱活性位点的单功能和双功能硅基介孔杂化催化剂的合成和表征。我们采用粉末 X 射线衍射、傅立叶变换红外光谱、多核 MAS NMR 光谱以及热重分析等多技术方法，对其协同催化能力进行了研究。为了阐明多功能催化位点的性质和强度，采用了不同类型的探针分子，并利用光谱技术对其进行了研究。结果表明，介孔表面接枝酸和/或碱位点的活性与亲和性标准，即不同类型催化位点之间的分离度直接相关。不同催化位点之间是否存在相互作用决定了反应的选择性和产率。
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