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Hydrolysis of ammonia borane for green hydrogen production over a Pd/C3N4 nanocatalyst synthesized by electron beam irradiation 利用电子束辐照合成的 Pd/C3N4 纳米催化剂水解氨硼烷以生产绿色氢气
IF 5 3区 化学
Catalysis Science & Technology Pub Date : 2024-09-18 DOI: 10.1039/d4cy00761a
Manish Shingole, Seemita Banerjee, Priyanka Ruz, Asheesh Kumar, Pratibha Sharma, V. Sudarsan
{"title":"Hydrolysis of ammonia borane for green hydrogen production over a Pd/C3N4 nanocatalyst synthesized by electron beam irradiation","authors":"Manish Shingole, Seemita Banerjee, Priyanka Ruz, Asheesh Kumar, Pratibha Sharma, V. Sudarsan","doi":"10.1039/d4cy00761a","DOIUrl":"https://doi.org/10.1039/d4cy00761a","url":null,"abstract":"Ammonia borane (AB), which possesses a theoretical hydrogen storage capacity of 19.6 wt%, is extensively examined to tackle solid state hydrogen storage challenges. In this paper, we present a strategy to synthesize Pd dispersed g-C<small><sub>3</sub></small>N<small><sub>4</sub></small> by decorating different concentrations of Pd on the g-C<small><sub>3</sub></small>N<small><sub>4</sub></small> matrix by electron beam irradiation process. Catalyst characterization reveals successful formation of g-C<small><sub>3</sub></small>N<small><sub>4</sub></small> supported highly dispersed face-centred cubic nanocrystalline Pd, with a particle size of less than 10 nm. The catalyst performance for AB hydrolysis exhibits an activation energy of 27.36 kJ mol<small><sup>−1</sup></small>, surpassing many Pd-based catalysts. Successive hydrolysis experiments and detailed analysis of the spent catalyst establish the reusability and stability of the catalyst. The study shows that though the initial AB concentration does not affect the hydrolysis reaction rate, addition of impurity ions to the reaction media can significantly modify it. Detailed mechanistic investigation by the kinetic isotope effect, time dependent FT-IR, and mass spectrometry clarifies that the evolved hydrogen from the AB hydrolysis reaction comes from both the breakage of the B–H bond and hydrogen from the solvent. Activation of the O–H bond of the solvent due to the adsorption on the catalyst surface plays a significant role in the AB hydrolysis reaction and comprises the rate-determining step.","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":null,"pages":null},"PeriodicalIF":5.0,"publicationDate":"2024-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142260022","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}
引用次数: 0
Single-step in situ synthesis of bimetallic catalysts via a gas-phase route: the case of PdZn–ZnO 通过气相路线原位一步合成双金属催化剂:PdZn-ZnO 案例
IF 5 3区 化学
Catalysis Science & Technology Pub Date : 2024-09-13 DOI: 10.1039/d4cy00807c
Andrija Kokanović, Dunja Pupavac, Stéphane Chenot, Stéphane Guilet, Igor M. Opsenica, Slavica Stankic
{"title":"Single-step in situ synthesis of bimetallic catalysts via a gas-phase route: the case of PdZn–ZnO","authors":"Andrija Kokanović, Dunja Pupavac, Stéphane Chenot, Stéphane Guilet, Igor M. Opsenica, Slavica Stankic","doi":"10.1039/d4cy00807c","DOIUrl":"https://doi.org/10.1039/d4cy00807c","url":null,"abstract":"In this study, we explore the catalytic activity of highly pure PdZn–ZnO nanopowder, synthesized <em>via</em> an innovative metal–organic chemical vapor synthesis (MOCVS) method. Unlike conventional methods that require post-synthesis treatments, this rapid, solvent-free synthesis produces a bimetallic nanocatalyst with a high surface area (<em>S</em><small><sub>BET</sub></small> ∼ 110 m<small><sup>2</sup></small> g<small><sup>−1</sup></small>) directly. X-ray diffraction (XRD) confirmed its high crystalline quality, identifying only PdZn-specific diffractions alongside the ZnO phase. High-resolution transmission electron microscopy (HRTEM) analysis revealed a single family of planes with an interplanar distance corresponding to PdZn (111) planes. Furthermore, X-ray photoelectron spectroscopy (XPS) and Fourier transform infrared spectroscopy using CO as a probe molecule (FTIR-CO), both conducted under ultra-high vacuum (UHV) conditions, unequivocally confirmed the presence of PdZn entities on the ZnO support. The catalytic performance of this one-step synthesized PdZn bimetallic catalyst was evaluated in the reduction of nitroarenes and hydrodebromination of arylbromides. The catalyst exhibited excellent activity in both reactions, with remarkable recyclability for the reduction of nitroarenes. Additionally, no significant decrease in yield was observed during scale-up tests. This study introduces a novel one-step approach for synthesizing bimetallic nanopowders, which can serve as highly active catalysts and model systems for surface science studies.","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":null,"pages":null},"PeriodicalIF":5.0,"publicationDate":"2024-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142260024","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}
引用次数: 0
The effect of polyunsaturation – insights into the hydroformylation of oleochemicals 多烯烃饱和度的影响--对油脂化学品加氢甲酰化的启示
IF 5 3区 化学
Catalysis Science & Technology Pub Date : 2024-09-12 DOI: 10.1039/d4cy00839a
Thomas Friedrich Hubertus Roth, Maximilian Lukas Spiekermann, David Lütkenhaus, Fabian Niefer, Dieter Vogt, Thomas Seidensticker
{"title":"The effect of polyunsaturation – insights into the hydroformylation of oleochemicals","authors":"Thomas Friedrich Hubertus Roth, Maximilian Lukas Spiekermann, David Lütkenhaus, Fabian Niefer, Dieter Vogt, Thomas Seidensticker","doi":"10.1039/d4cy00839a","DOIUrl":"https://doi.org/10.1039/d4cy00839a","url":null,"abstract":"Although the hydroformylation of vegetable oil-derived oleochemicals, such as methyl oleate, is a highly demanded reaction and has been intensively studied, little is known about the influence of naturally occurring polyunsaturated (PU) components and their effect on the homogeneous rhodium catalyst. This is now examined in detail in the presented work by conducting systematic perturbation experiments. For the first time, it can be verified that the isomerisation of double bonds in polyunsaturated oleochemicals generates conjugated double bond systems that form stable η<small><sup>3</sup></small>-Rh allyl species and thus temporarily inhibit the catalyst. However, based on these findings, hydroformylation activity can be significantly increased by selective hydrogenation of PU to monounsaturated components. In the case of sunflower methyl ester, the turnover frequency multiplied by a factor of 8 and reached 3201 h<small><sup>−1</sup></small>, the highest rate reported in the context of methyl oleate hydroformylation. These effects were shown for both phosphine and phosphite ligands under both mono- and biphasic conditions and for methyl esters with different PU content, stressing the magnitude of this effect. This work makes it possible to support long-observed phenomena with the underlying mechanism scientifically. This lays the scientific basis for efficiently converting oleochemicals into valuable intermediates through hydroformylation for an increased share of renewable carbon in the chemical value chain.","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":null,"pages":null},"PeriodicalIF":5.0,"publicationDate":"2024-09-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142260025","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}
引用次数: 0
Exploring the impact of abnormal coordination in macrocyclic N-heterocyclic carbene ligands on bio-inspired iron epoxidation catalysis 探索大环 N-杂环碳烯配体的异常配位对生物启发铁环氧化催化的影响
IF 5 3区 化学
Catalysis Science & Technology Pub Date : 2024-09-12 DOI: 10.1039/d4cy00992d
Greta G. Zámbó, Carla A. Esslinger, Michael J. Sauer, Isabelle Rüter, Robert M. Reich, Serhiy Demeshko, Franc Meyer, Fritz E. Kühn
{"title":"Exploring the impact of abnormal coordination in macrocyclic N-heterocyclic carbene ligands on bio-inspired iron epoxidation catalysis","authors":"Greta G. Zámbó, Carla A. Esslinger, Michael J. Sauer, Isabelle Rüter, Robert M. Reich, Serhiy Demeshko, Franc Meyer, Fritz E. Kühn","doi":"10.1039/d4cy00992d","DOIUrl":"https://doi.org/10.1039/d4cy00992d","url":null,"abstract":"The first macrocyclic abnormal <em>N</em>-heterocyclic carbene (aNHC) Fe<small><sup>III</sup></small> complex, featuring a calix[4]3-methyl-1,2,3-triazole-5-ylidene ligand system is synthesised and characterised <em>inter alia via</em> EA, SC-XRD, NMR and UV/vis spectroscopy. Including Mössbauer spectroscopy, SQUID and DFT calculations, the impact of the aNHC on the Fe<small><sup>III</sup></small> complex and its corresponding Fe<small><sup>II</sup></small> derivative is investigated. A comprehensive study of the aNHC Fe complexes in their performance in homogenous epoxidation reactions is reported and compared to the established benchmark catalysts. The complexes demonstrate efficient and selective catalytic activity in the epoxidation of <em>cis</em>-cyclooctene with H<small><sub>2</sub></small>O<small><sub>2</sub></small>, with TOFs up to almost 60 000 h<small><sup>−1</sup></small>. Additionally, the epoxidation of more challenging olefinic substrates is possible. The reactivity under oxidative conditions of both complexes is investigated. NMR measurements reveal the formation of a mono-oxidised triazole ligand as degradation product. HR-ESI-MS measurements, supported by DFT calculations indicate the formation of an oxoiron species.","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":null,"pages":null},"PeriodicalIF":5.0,"publicationDate":"2024-09-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142260026","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}
引用次数: 0
Selective CO production from CO2 over a metal catalyst supported on perovskite oxide in the presence of excess hydrogen 在过量氢气存在的情况下,以过氧化物为支撑的金属催化剂从 CO2 中选择性地生产 CO
IF 5 3区 化学
Catalysis Science & Technology Pub Date : 2024-09-11 DOI: 10.1039/d4cy00797b
Keigo Tashiro, Shinnosuke Sekizawa, Wataru Doi, Hikaru Konno, Kensuke Izutani, Takayuki Furukawa, Akihide Yanagita, Shigeo Satokawa
{"title":"Selective CO production from CO2 over a metal catalyst supported on perovskite oxide in the presence of excess hydrogen","authors":"Keigo Tashiro, Shinnosuke Sekizawa, Wataru Doi, Hikaru Konno, Kensuke Izutani, Takayuki Furukawa, Akihide Yanagita, Shigeo Satokawa","doi":"10.1039/d4cy00797b","DOIUrl":"https://doi.org/10.1039/d4cy00797b","url":null,"abstract":"Hydrogenation of carbon dioxide (CO<small><sub>2</sub></small>) to liquid fuels <em>via</em> an industrial catalytic reaction is the most effective strategy for the realization of carbon neutrality. The sequential reaction system of a reverse water–gas shift (RWGS) reaction followed by Fischer–Tropsch synthesis is a promising way to achieve this; hence, the development of catalysts with high conversion efficiency and selectivity for RWGS is required. We succeeded in the conversion of CO<small><sub>2</sub></small> into carbon monoxide (CO) with a selectivity of 100% in the gas phase using a platinum-loaded perovskite oxide support composed of barium and zirconium, in which 10% of zirconium was substituted with yttrium (Pt/BaZr<small><sub>0.9</sub></small>Y<small><sub>0.1</sub></small>O<small><sub>3−<em>δ</em></sub></small>, Pt/BZY10) at 500 °C in the gas stream with H<small><sub>2</sub></small>/CO<small><sub>2</sub></small> = 3. Furthermore, a ruthenium-loaded catalyst (Ru/BZY10) afforded not only CO but also methane (CH<small><sub>4</sub></small>) as gaseous products. Kinetic analysis demonstrated that the activation energy was identical for both catalysts, and Fourier transform infrared spectroscopy clarified that the surface-adsorbed methoxy group was generated as a reaction intermediate only in the case of Ru/BZY10, which indicated the ability of the loaded metal for the dissociative adsorption of hydrogen. The present research is expected to provide a new methodology for the preparation of catalysts for the RWGS reaction and a quite important insight for the realization of carbon neutrality.","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":null,"pages":null},"PeriodicalIF":5.0,"publicationDate":"2024-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142205460","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}
引用次数: 0
High temperature reductive treatment promotes thermal stability of Pt/hexaaluminate catalysts for CO and C3H8 oxidation 高温还原处理提高了用于 CO 和 C3H8 氧化的铂/六铝酸盐催化剂的热稳定性
IF 5 3区 化学
Catalysis Science & Technology Pub Date : 2024-09-11 DOI: 10.1039/d4cy00708e
Yumeng Xu, Rongzhou Chen, Hailian Tang, Lu Yan, Fei Huang, Ming Tian, Kaibao Wu, Yanliang Zhou, Jian Lin, Ying Zheng, Xiaodong Wang
{"title":"High temperature reductive treatment promotes thermal stability of Pt/hexaaluminate catalysts for CO and C3H8 oxidation","authors":"Yumeng Xu, Rongzhou Chen, Hailian Tang, Lu Yan, Fei Huang, Ming Tian, Kaibao Wu, Yanliang Zhou, Jian Lin, Ying Zheng, Xiaodong Wang","doi":"10.1039/d4cy00708e","DOIUrl":"https://doi.org/10.1039/d4cy00708e","url":null,"abstract":"Promoting the thermal stability of supported noble metal catalysts under harsh conditions remains challenging for the modern chemistry industry. Herein, Fe-substituted hexaaluminate supported Pt catalysts (Pt/BaFeAl<small><sub>11</sub></small>O<small><sub>19</sub></small>) were synthesized and treated with high temperature at 800 °C under different atmospheres. The Pt particles showed severe sintering under an oxidative atmosphere but high stability under reductive conditions. Interestingly, Pt/BaFeAl<small><sub>11</sub></small>O<small><sub>19</sub></small> pre-reduced at high temperature possessed improved anti-sintering ablility during oxidative annealing. The characterization results demonstrate that oxygen vacancies were facilely formed under an H<small><sub>2</sub></small> atmosphere to favor the formation of coating layers on Pt nanoparticles. This structure helps retain oxygen vacancies during subsequent oxidative calcination, contributing to promoted stability. The high thermal stability of Pt particles coupled with the easy generation of Fe<small><sup>2+</sup></small> sites in Pt/BaFeAl<small><sub>11</sub></small>O<small><sub>19</sub></small> resulted in excellent catalytic performance for CO and C<small><sub>3</sub></small>H<small><sub>8</sub></small> oxidation after cycling hydrothermal aging at 800 °C.","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":null,"pages":null},"PeriodicalIF":5.0,"publicationDate":"2024-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142226296","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}
引用次数: 0
Selective catalytic NOx reduction by H2 in excess O2 over Pt/zirconium phosphate nanosheets 磷酸铂/锆纳米片在过量氧气中利用 H2 选择性催化还原氮氧化物
IF 5 3区 化学
Catalysis Science & Technology Pub Date : 2024-09-11 DOI: 10.1039/d4cy00879k
Keisuke Awaya, Yuka Sato, Aoi Miyazaki, Mana Furukubo, Koshi Nishiyama, Masayuki Tsushida, Shintaro Ida, Junya Ohyama, Masato Machida
{"title":"Selective catalytic NOx reduction by H2 in excess O2 over Pt/zirconium phosphate nanosheets","authors":"Keisuke Awaya, Yuka Sato, Aoi Miyazaki, Mana Furukubo, Koshi Nishiyama, Masayuki Tsushida, Shintaro Ida, Junya Ohyama, Masato Machida","doi":"10.1039/d4cy00879k","DOIUrl":"https://doi.org/10.1039/d4cy00879k","url":null,"abstract":"Two-dimensional nanomaterials have attracted attention over the past several decades in the field of catalyst materials chemistry because of their intrinsic anisotropic crystal structure and large specific surface area. In particular, transition-metal phosphate (TMP) nanosheets have great potential as supporting materials for platinum-group metal (PGM) catalysts for the conversion of NO <em>via</em> selective catalytic reduction (SCR). A previous report concluded that the Rh/ZrP<small><sub>2</sub></small>O<small><sub>7</sub></small> catalyst showed good catalytic activity in the SCR reaction with C<small><sub>3</sub></small>H<small><sub>6</sub></small> due to the strong anchoring effect of Rh–O–P linkages and the electrophilic nature of PO<small><sub>4</sub></small>, which surpasses sintering of RhO<small><sub><em>x</em></sub></small> nanoparticles and promotes the rapid redox reactions of Rh species. In the present study, we demonstrated the catalytic activity toward NO conversion <em>via</em> SCR with H<small><sub>2</sub></small> (H<small><sub>2</sub></small>-SCR) using Pt nanoparticles supported on a monolayer zirconium phosphate (ZrP) nanosheet. The monolayer ZrP nanosheet was obtained by delaminating layered alpha-zirconium phosphate (α-Zr(HPO<small><sub>4</sub></small>)<small><sub>2</sub></small>·H<small><sub>2</sub></small>O) in 0.25 M ethylamine solution (50% ethanol in water). The crystal structure of the ZrP nanosheet was thermally stable upto 500 °C after the Zr(HPO<small><sub>4</sub></small>)<small><sub>2</sub></small> was transformed into ZrP<small><sub>2</sub></small>O<small><sub>7</sub></small>, which was a sufficiently high temperature for operation as an H<small><sub>2</sub></small>-SCR catalyst (RT-400 °C). The 0.49 wt% Pt/ZrP nanosheet showed high NO conversion (89%) and moderate N<small><sub>2</sub></small> selectivity (83%) at 150 °C under a NO (200 ppm)–H<small><sub>2</sub></small> (5000 ppm)–O<small><sub>2</sub></small> (10%)–He (balance) atmosphere. The Pt/ZrP nanosheet catalyst maintained its catalytic activity when the H<small><sub>2</sub></small>-SCR test was repeated for three cycles. Further investigation of the particle size (HAADF-STEM) and electronic state (XPS) of the Pt suggested that the small Pt particles (diameter: ∼1 nm) with a high loading amount on the ZrP nanosheet structure were key to achieving a high NO conversion rate with a low yield of NO<small><sub><em>x</em></sub></small> byproducts.","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":null,"pages":null},"PeriodicalIF":5.0,"publicationDate":"2024-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142205438","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}
引用次数: 0
Arsenene/PtO2 heterojunction: a potential Z-scheme photocatalyst with tunable electronic properties and efficient catalytic activity 砷/二氧化铂异质结:具有可调电子特性和高效催化活性的潜在 Z 型光催化剂
IF 5 3区 化学
Catalysis Science & Technology Pub Date : 2024-09-11 DOI: 10.1039/d4cy00681j
Wentao Luo, Jiaxin Wang, Xing Wei, Yan Zhang, Yun Yang, Jian Liu, Ye Tian, Ziyuan Li, Shijie Wei, Li Duan
{"title":"Arsenene/PtO2 heterojunction: a potential Z-scheme photocatalyst with tunable electronic properties and efficient catalytic activity","authors":"Wentao Luo, Jiaxin Wang, Xing Wei, Yan Zhang, Yun Yang, Jian Liu, Ye Tian, Ziyuan Li, Shijie Wei, Li Duan","doi":"10.1039/d4cy00681j","DOIUrl":"https://doi.org/10.1039/d4cy00681j","url":null,"abstract":"This paper systematically investigates the geometric composition, electronic behavior and photocatalytic performance of arsenene/PtO<small><sub>2</sub></small> heterojunctions through computational studies grounded in the principles of density functional theory (DFT). This study demonstrates that the arsenene/PtO<small><sub>2</sub></small> heterojunction exhibits a typical type II band alignment with an indirect bandgap narrowed to 1.43 eV. The Z-scheme charge transfer mechanism is more conducive to the separation of photogenerated carriers to promote catalytic reactions. Moreover, the band edge positions of the arsenene/PtO<small><sub>2</sub></small> heterojunction are capable of surpassing the redox potential of water across a range of pH conditions. Hydrogen is generated on the conduction band (CB) of arsenene during the reduction process, while the valence band (VB) of PtO<small><sub>2</sub></small> hosts the oxidation process that produces oxygen, collectively driving water splitting. At the same time, under compressive and tensile strains of 0–6%, the band edge alignment of the arsenene/PtO<small><sub>2</sub></small> heterojunction still meets the requirements for photocatalytic water splitting. Moreover, the arsenene/PtO<small><sub>2</sub></small> heterojunction not only exhibits enhanced light absorption capabilities compared to the individual monolayer materials but also demonstrates improved light absorption performance under tensile strain, and its solar-to-hydrogen (STH) efficiency reaches 47.29%. Consequently, the arsenene/PtO<small><sub>2</sub></small> heterojunction is expected to become a strong candidate material for the next generation of photocatalysts.","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":null,"pages":null},"PeriodicalIF":5.0,"publicationDate":"2024-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142205436","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}
引用次数: 0
Sulfonic acid-modified MOFs as heterogeneous bifunctional catalysts for ethylene oligomerization at room temperature without cocatalysts 磺酸修饰的 MOFs 作为异相双功能催化剂,用于室温下乙烯低聚而无需助催化剂
IF 5 3区 化学
Catalysis Science & Technology Pub Date : 2024-09-11 DOI: 10.1039/d4cy00502c
Yao Ning, Yuqi Yang, Dongming Shan, Shuxing Mei, Yibai Yan, Linjie Ding, Ying Zhang
{"title":"Sulfonic acid-modified MOFs as heterogeneous bifunctional catalysts for ethylene oligomerization at room temperature without cocatalysts","authors":"Yao Ning, Yuqi Yang, Dongming Shan, Shuxing Mei, Yibai Yan, Linjie Ding, Ying Zhang","doi":"10.1039/d4cy00502c","DOIUrl":"https://doi.org/10.1039/d4cy00502c","url":null,"abstract":"Ethylene oligomerization plays an important role in industrial production. However, when taking the traditional non-metallocene catalysts and MOF catalysts for ethylene oligomerization, they typically require methylaluminoxane (MAO), aluminum alkyl, and other cocatalysts, which is neither environmentally friendly nor helpful in reducing production costs. Here, three sulfonic acid-modified MOFs (SA/MIL-101(Cr), UiO-66-NS and MIL-101(Cr)-NS) were prepared and used as catalysts for ethylene oligomerization at room temperature without using any cocatalysts. All of them exhibited excellent catalytic performances (<em>e.g.</em>, 10SA/MIL-101(Cr), 21 953 g mol<small><sub>Cr</sub></small><small><sup>−1</sup></small> h<small><sup>−1</sup></small>, with C<small><sub>8</sub></small> selectivity greater than 70.32%), and their oligomerization activity increased by almost tenfold compared to unmodified MOFs. The presence of Lewis acid (L acid) and Brønsted acid (B acid) sites in modified MOFs is the key to improved performances. In particular, the presence of B acid weakens the role of metal clusters and ligands in MOFs, making it easier for metal centers to bind to ethylene molecules for further oligomerization. This work first demonstrates that bifunctional MOF catalysts can catalyze ethylene tetramerization under mild conditions without cocatalysts.","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":null,"pages":null},"PeriodicalIF":5.0,"publicationDate":"2024-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142260047","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}
引用次数: 0
Accelerated design of nickel-cobalt based catalysts for CO2 hydrogenation with human-in-the-loop active machine learning 利用人在回路中的主动机器学习加速设计二氧化碳加氢用镍钴基催化剂
IF 5 3区 化学
Catalysis Science & Technology Pub Date : 2024-09-10 DOI: 10.1039/d4cy00873a
Yasemen Kuddusi, Maarten R. Dobbelaere, Kevin M. Van Geem, Andreas Züttel
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