Catalysis Science & Technology最新文献

{"title":"Rational reconstruction from attapulgite to MCM-41 and its superior application in formaldehyde degradation†","authors":"Dan Chen ,&nbsp;Jing Zhang ,&nbsp;Ming Zhai ,&nbsp;Xin Chen ,&nbsp;Liqi Miao ,&nbsp;Kan Li ,&nbsp;Zhong Wang ,&nbsp;Xiaozhi Wang","doi":"10.1039/d4cy01203h","DOIUrl":"10.1039/d4cy01203h","url":null,"abstract":"<div><div>The inferior reactive metal dispersion caused by a lack of structural defects limits the application of MCM-41 in synthesizing effective catalysts. Herein, we substituted a conventional silicon source (TEOS) with attapulgite to fabricate structural defects on MCM-41. Catalytic performance evaluation results after Ag incorporation proved that this substitution favored HCHO degradation. It was observed that owing to their high structural stability, attapulgite rods only merged with each other during MCM-41 construction, which resulted in a sheet-like morphology without the formation of any mesoporous structure. Notably, the metal species (Al, Mg and Fe) in attapulgite improved the dispersion and size distribution of Ag nanoparticles and intensified the electronic properties of Ag species. As for MCM-41 prepared with acidified attapulgite, demetallization resulted in the exposure of Si–O⁻ groups and a decrease in structural stability. In subsequent MCM-41 construction, acidified attapulgite collapsed into colloidal particles and debris. Further, the colloidal particles were drawn together by CTA⁺, leading to the formation of chrysalis-like particles with regular mesopores, and debris that surrounded CTA⁺ collapsed, forming cotton-like morphology with irregular mesopores. Notably, the reservation of Si–O⁻ groups after MCM-41 construction could enhance the exposure of oxygen species and the dispersion of Ag nanoparticles on the outer surface and inner mesopores. Moreover, such Si–O⁻ groups are adsorptive and reactive towards HCHO.</div></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"15 7","pages":"Pages 2186-2201"},"PeriodicalIF":4.4,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143740488","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Unveiling a carbazole-based photocatalyst for visible-light-driven synthesis of indolyl diarylmethanes and 2-benzimidazoles†","authors":"Sunil Kumar ,&nbsp;K. R. Justin Thomas","doi":"10.1039/d5cy00043b","DOIUrl":"10.1039/d5cy00043b","url":null,"abstract":"<div><div>A carbazole-based photocatalyst (MD) incorporating a dicyanovinyl acceptor and exhibiting superior redox potential has been demonstrated for a sustainable photocatalytic approach to synthesize indolyl diarylmethanes and 2-substituted benzimidazoles. This protocol operates <em>via</em> an oxidative quenching cycle of MD under visible light, eliminating the need for external oxidants or metal catalysts. The methodology offers excellent functional group tolerance, high selectivity, and environmentally friendly conditions, making it a valuable contribution to green photocatalysis.</div></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"15 7","pages":"Pages 2143-2147"},"PeriodicalIF":4.4,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143740469","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"The effects of SO2 impurities on CO2 electroreduction on bare silver and SiO2 coated silver in different cell geometries†","authors":"Ming Li ,&nbsp;Shilong Fu ,&nbsp;Ruud Kortlever ,&nbsp;J. Ruud van Ommen","doi":"10.1039/d4cy01196a","DOIUrl":"10.1039/d4cy01196a","url":null,"abstract":"<div><div>Electrochemical CO₂ reduction presents an opportunity to transform waste flue gas with water and renewable electricity into chemicals or fuels. However, the energy-intensive nature of purification of flue gas underscores the appeal of directly utilizing the flue gas streams containing impurities. In this study, we investigate the impact of SO₂ impurities on CO₂ electroreduction in two electrochemical cell geometries: an H-cell and a membrane electrode assembly (MEA) cell. We observe distinctly different behavior of the Ag on carbon black (Ag/CB) catalyst under SO₂ impurities in the H-cell compared to the MEA cell, where SO₂ impurities exhibit a more pronounced effect on Ag/CB catalysts in the H-cell than in the MEA cell. This difference is attributed to the higher solubility of SO₂ in the electrolyte compared to CO₂, resulting in an accumulation effect and causing differences in the SO₂ concentration near the electrode between the H-cell and the MEA system. By depositing a very thin SiO₂ coating on the outermost surface of the Ag/CB catalyst using atomic layer deposition (ALD), the impact of SO₂ on the catalyst's selectivity is diminished. This is attributed to the permeability difference between CO₂ and SO₂ through the SiO₂ coatings and results in a local SO₂ concentration difference between samples with and without SiO₂ coatings.</div></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"15 7","pages":"Pages 2148-2159"},"PeriodicalIF":4.4,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/cy/d4cy01196a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143740470","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"CO2 electroreduction towards ethylene on copper phosphate-derived catalysts in alkaline flow cell†","authors":"Julien K. Dangbegnon ,&nbsp;Marco Etzi ,&nbsp;Juqin Zeng ,&nbsp;Angelica Chiodoni ,&nbsp;Candido F. Pirri","doi":"10.1039/d4cy01365d","DOIUrl":"10.1039/d4cy01365d","url":null,"abstract":"<div><div>CO₂ electroreduction into valuable hydrocarbons with high selectivity is of high market interest yet challenging. Cu-based catalysts have a unique catalytic activity toward hydrocarbon products in the CO₂ electroreduction reaction. They are widely studied to promote the corresponding selectivity and activity. The control of the oxidation state of the catalyst is essential in driving the reaction toward the desired hydrocarbon. Herein, we steer CO₂ electroreduction toward ethylene production with high selectivity in an alkaline flow cell configuration from a copper phosphate catalyst. An optimum faradaic efficiency of 55% for ethylene was obtained in a 7 M KOH electrolyte at a total current density of 150 mA cm⁻². The investigation of the mechanism shows that Cu nanoparticles are derived during electrolysis, which may favour the dimerisation of *CO to ethylene formation. This work provides new insights into designing catalysts for high-selectivity hydrocarbon formation.</div></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"15 7","pages":"Pages 2318-2326"},"PeriodicalIF":4.4,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143740507","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Efficient CO2 reduction to methane on Ru2-based adjacent vacant graphene catalysts: insights into bimetallic synergies, thermodynamics, and kinetics†","authors":"Anand Mohan Verma ,&nbsp;Nanda Kishore","doi":"10.1039/d5cy00005j","DOIUrl":"10.1039/d5cy00005j","url":null,"abstract":"<div><div>Electrochemical conversion of CO₂ into value-added chemicals offers a clean pathway to utilize greenhouse gases along with the production of useful products. In this study, we aim to unravel a comprehensive reaction mechanism for the CO₂ reduction reaction (CO₂RR) into various C₁-based products such as CO, HCOOH, CH₂O, CH₃OH, and CH₄ using density functional theory (DFT). We analyse all possible reaction pathways and compute their thermodynamics on a novel two-dimensional catalyst system – two monovacant (adjacent-vacant) graphene sheet modified with two Ru atoms, referred to as 2MV-Ru₂. Our reaction mechanism investigation identified the potential-determining step (PDS) as CO* → CHO*, which demands a limiting potential of −0.88 V <em>vs.</em> SHE (standard hydrogen electrode) for the production of methane. We also examined the PDS on a series of bimetallic electrodes, generally referred to as 2MV-RuM (M = Ag, Au, Cu, Ir, Os, Pd, Pt, and Rh). We found the 2MV-RuPd electrode as the most effective catalyst for methane production as it lowered the limiting potential of PDS to only −0.13 V <em>vs.</em> SHE, which is a remarkable improvement over both 2MV-Ru₂ and conventional metallic electrodes. To supplement the thermodynamics, we also integrated kinetic analyses for the PDS to provide a more inclusive understanding of the reaction, which demonstrated the excellent capability of 2MV-RuPd electrode compared to 2MV-Ru₂. Finally, we examined the stability of all bimetallic electrodes to ensure their practical applicability, and obtained favourable formation free energies, which advocate that these electrodes are not only theoretically feasible but also experimentally synthesizable. Overall, our study offers a rigorous analysis of the CO₂RR on Ru-based adjacent-vacant (bimetallic) graphene catalysts. Superior thermodynamics and kinetics were demonstrated by the 2MV-RuPd electrode, thereby establishing it as a highly promising candidate for methane production. This work advances the understanding of CO₂RR mechanisms along with providing a robust foundation for developing next-generation catalysts for sustainable chemical synthesis.</div></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"15 7","pages":"Pages 2379-2394"},"PeriodicalIF":4.4,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143740512","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"NiPt catalysts for the synthesis of iso-butanol: the influence of molar ratio and total metal loading on activity and stability†","authors":"Joachim Pasel ,&nbsp;Johannes Häusler ,&nbsp;Ralf Peters ,&nbsp;Detlef Stolten","doi":"10.1039/d5cy00078e","DOIUrl":"10.1039/d5cy00078e","url":null,"abstract":"<div><div>If methanol and ethanol are produced regeneratively from green H₂ and CO₂, a mixture of these two can further react to form longer-chain branched alcohols such as iso-butanol, which can serve as sustainable feedstocks for the transportation and chemical sectors. NiPt catalysts have shown to be promising for this process. This study investigates the influence of the total metal loading Ni + Pt and the molar ratio of Ni to Pt on catalytic behavior. It was observed that the values for the total metal loading and the molar fraction of Pt must be set correctly and precisely during synthesis, as most of all the space–time yield of the catalyst, the conversion of ethanol, and the iso-butanol yield strongly depend on them. Differing mechanisms for the decomposition of acetaldehyde on pure Pt/C and NiPt/C are comparatively discussed. They explain the beneficial effect of Ni in avoiding the formation of carbonaceous deposits on the active centers. In addition, Ni was found to prevent particle growth due to its strong metal–support interaction.</div></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"15 7","pages":"Pages 2248-2260"},"PeriodicalIF":4.4,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/cy/d5cy00078e?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143740434","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Insight into the Co and N statuses in MOF-derived porous carbonaceous materials in catalytic ozonolysis at room temperature†","authors":"Kun Wang ,&nbsp;Binglin Xin ,&nbsp;Runduo Zhang ,&nbsp;Zhaoying Di ,&nbsp;Bin Kang ,&nbsp;Xiaonan Guo ,&nbsp;Ying Wei ,&nbsp;Jingbo Jia ,&nbsp;Zhou-jun Wang","doi":"10.1039/d4cy01468e","DOIUrl":"10.1039/d4cy01468e","url":null,"abstract":"<div><div>Ozone is one of the classical atmospheric pollutants that adversely affects human health and the ecological environment. In this paper, carbonaceous catalysts derived from MOFs with different structural topologies and organic ligands were systematically investigated for ozone elimination. Upon carbonization, ZIF-67-NC was formed with a rich microporous structure and N doping in the corresponding carbon support. N doping facilitated the further dispersion and redox behavior of the active Co²⁺ cations. Moreover, the high nitrogen content promoted the formation of more defective sites in ZIF-67-NC, which can facilitate the formation of Co–N structure and bring the highest content of these active centers. Furthermore, a large number of microporous structures is beneficial for the exposed Co–N active sites and enhanced the O₃ adsorption, leading to a better activity and stability. The ZIF-67-NC exhibited an ozone conversion close to 100% at a concentration of 40 ppm O₃ and 50% relative humidity for 16 h. <em>In situ</em> DRIFTs and theoretical calculations confirmed the excellent capacity for O₂²⁻ and O₂⁻ desorption of ZIF-67-NC. The lowest energy barrier and weakest O₂ adsorption strength enabled an efficient O₃ decomposition and successive O₂ desorption.</div></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"15 7","pages":"Pages 2202-2220"},"PeriodicalIF":4.4,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143740489","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Design and catalytic performance investigation of the Ni–N–C catalyst for CO2RR: a theoretical study†","authors":"Yiming Sun ,&nbsp;Xiaoyu Wang ,&nbsp;Zhuofan Wu ,&nbsp;Anmin Liu ,&nbsp;Xuefeng Ren","doi":"10.1039/d4cy01394h","DOIUrl":"10.1039/d4cy01394h","url":null,"abstract":"<div><div>The combustion of fossil fuels is increasingly contributing to global warming. The recycling of CO₂ plays a crucial role, and the creation of a highly efficient electrocatalyst is essential for enhancing the efficiency of the reaction. This work focused on the theoretical design of Ni–N–C catalysts with different coordination environments of Ni through quantum chemical calculations and analyzed the differences between the coordination environments of pyridine N and pyrrole N on the performance of catalytic CO₂ reduction to CO in order to identify the most efficient catalyst configuration. The Ni–N bonding energy of the catalyst with a vacancy was greater than that of the catalyst without a vacancy, and the activation ability of Ni-pyridine N₂C₁–C was the best. Ultimately, examining various catalysts for converting CO₂ into CO revealed that Ni-pyridine N₂C₁–C exhibited the most effective catalytic impact. In contrast to the energy barrier Δ<em>G</em> = 2.9903 eV in the absence of a catalyst, the energy barrier Δ<em>G</em> = −1.4029 eV during the CO₂ to CO catalytic reaction decreased by 4.3932 eV. This decrease was the largest among all the catalysts mentioned above, and the reaction could be spontaneous from a thermodynamic perspective. The research results provide a theoretical reference for the experimental preparation of catalysts for CO₂ to CO conversion and the resource utilization of CO₂.</div></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"15 7","pages":"Pages 2175-2185"},"PeriodicalIF":4.4,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/cy/d4cy01394h?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143740472","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"One-dimensional gold-doped monoclinic iridium oxide nanoribbons for high-efficiency acidic oxygen evolution reaction†","authors":"Hanzhuo Luo ,&nbsp;Sihui Pan ,&nbsp;Chenchen Li ,&nbsp;Penghao Li ,&nbsp;Jia Ke ,&nbsp;Yue Wang ,&nbsp;Long Chen ,&nbsp;Qi Shao","doi":"10.1039/d5cy00014a","DOIUrl":"10.1039/d5cy00014a","url":null,"abstract":"<div><div>Proton exchange membrane water electrolysis (PEMWE) stands as the predominant technique for the production of high-purity hydrogen. However, it is confronted with a significant impediment due to the sluggish kinetics inherent to the anodic oxygen evolution reaction (OER). This limitation has spurred the search for catalysts that exhibit both high activity and durability in facilitating the OER. One-dimensional (1D) metastable-phase iridium oxide (IrO₂) has emerged as a promising OER catalyst, yet its catalytic activity and stability have hitherto fallen short of the stringent requirements for industrial-scale applications. Here, by leveraging a heteroatom doping strategy, we have successfully synthesized 1D gold-doped IrO₂ monoclinic nanoribbons (Au-doped IrO₂NRs), further optimizing the electrochemical activity and durability of IrO₂ nanoribbons under acidic conditions. Au-doped IrO₂NRs not only preserve the crystal structure characteristic of monoclinic IrO₂NRs, but also exhibit improved catalytic performance. Under an acidic environment, Au-doped IrO₂NRs reach a low overpotential of 180 mV at a current density of 10 mA cm⁻², a low Tafel slope of 40.6 mV dec⁻¹, and a durable stability of 160 h at 10 mA cm⁻². When integrating into the anode compartment of a practical PEMWE system, Au-doped IrO₂NRs sustained operation for more than 500 h at 60 °C. These results highlight the capacity of Au-doped IrO₂NRs to promote the performance and endurance of PEMWE, which in turn supports the wider implementation of hydrogen as a sustainable energy carrier.</div></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"15 7","pages":"Pages 2221-2228"},"PeriodicalIF":4.4,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143740490","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Na-decorated binary spinel ferrite catalysts for the hydrogenation of CO2 to olefins†","authors":"Hanjun Lu ,&nbsp;Xia Li ,&nbsp;Guangchao Li ,&nbsp;Xinlin Hong ,&nbsp;Shik Chi Edman Tsang","doi":"10.1039/d5cy00033e","DOIUrl":"10.1039/d5cy00033e","url":null,"abstract":"<div><div>Spinel ferrite catalysts, recognized for their unique physicochemical properties, have been extensively employed in CO₂ hydrogenation reactions. However, the specific roles of different transition metals in Na-decorated spinel ferrite for CO₂ hydrogenation to olefins remain underexplored. In this study, we designed a series of Na-decorated binary spinel ferrites by varying the type of the secondary metals. We found that doping with zinc reduces the hydrogenation ability, which enhances olefin selectivity. Conversely, adding copper facilitates catalyst reduction through H₂-spillover, with the CuFe interface increasing alcohol products. CoFe₂O₄ demonstrated the highest activity and olefin yield. Additionally, CoFe₂O₄ was found to promote the formation of the carbide phase and enhance the activation and dissociation of hydrogen, significantly boosting catalytic performance. Our findings pave the way for developing Na-decorated spinel catalysts tailored for selective olefin synthesis, with important implications for improving the efficiency of CO₂ hydrogenation processes.</div></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"15 7","pages":"Pages 2229-2237"},"PeriodicalIF":4.4,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/cy/d5cy00033e?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143740491","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}