Catalysis Science & Technology最新文献

{"title":"Insight into the influence of Re and Cl on Ag catalysts in ethylene epoxidation.","authors":"Claudia J Keijzer, Pim T Weide, Kristiaan H Helfferich, Justyna Zieciak, Marco de Ridder, Remco Dalebout, Tracy L Lohr, John R Lockemeyer, Peter van den Brink, Petra E de Jongh","doi":"10.1039/d4cy00858h","DOIUrl":"10.1039/d4cy00858h","url":null,"abstract":"<p><p>Commercial ethylene epoxidation catalysts consist of α-alumina supported Ag particles and usually contain a mixture of promoters. High selectivity catalysts typically include a small amount of rhenium species. We studied a series of Ag catalysts promoted with Re loadings up to 4 at% (Re/(Re + Ag)), which is intentionally higher than in optimized commercial catalysts to facilitate characterization and to amplify the influence on catalysis. Sequential impregnation brought Re and Ag in such close contact that they formed a new characterized phase of AgReO₄. Chemisorption experiments showed that both ReO _<i>x</i> and AgReO₄ species act as a reversible reservoir for O₂. Ethylene epoxidation was performed without and with the industrially crucial ethyl chloride promoter in the feed. Without the chloride (Cl), the ethylene oxide selectivity increased when Re was present, whereas the combination of Re and Cl decreased the ethylene oxide selectivity at higher Re loadings. Systematic ethylene oxide isomerization experiments revealed that Re and Cl individually inhibit the isomerization on the Ag surface. However, Re and Cl combined increased the isomerization, which can be explained by the surface becoming overly electrophilic. This hence shows the importance of studying promoters both individually and combined.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" ","pages":""},"PeriodicalIF":4.4,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11563198/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142646022","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":"Correction: Design of gold catalysts for activation of H2 and H-donor molecules: transfer hydrogenation and CO2 hydrogenation","authors":"Jhonatan Luiz Fiorio, Lais Reis Borges, Tomaz Neves-Garcia, Danielle Kimie Kikuchi, Raíza Rosa Garcia Guerra and Liane Marcia Rossi","doi":"10.1039/D3CY90065G","DOIUrl":"https://doi.org/10.1039/D3CY90065G","url":null,"abstract":"<p >Correction for ‘Design of gold catalysts for activation of H<small>₂</small> and H-donor molecules: transfer hydrogenation and CO<small>₂</small> hydrogenation’ by Jhonatan Luiz Fiorio <em>et al.</em>, <em>Catal. Sci. Technol.</em>, 2023, <strong>13</strong>, 3205–3215, https://doi.org/10.1039/D2CY01920E.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 18","pages":" 5462-5463"},"PeriodicalIF":5.0,"publicationDate":"2023-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2023/cy/d3cy90065g?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"7164191","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":"Hierarchical hollow TiO2/In2S3 heterojunction photocatalyst decorated with spatially separated dual co-catalysts for enhanced photocatalytic H2 evolution†","authors":"Ruyu Zhang, Xiaowei Jia, Xianchun Liu, Mingliang Sun, Yuyu Wang, Anqi Xie, Xiaodan Yu, Zhan Shi and Yan Xing","doi":"10.1039/D3CY00838J","DOIUrl":"https://doi.org/10.1039/D3CY00838J","url":null,"abstract":"<p >Achieving enhanced charge separation efficiency and accelerated surface reaction kinetics are crucial for high-performance photocatalytic hydrogen evolution. Herein, a spatially separated, dual co-catalyst-modified photocatalytic system Pt/TiO<small>₂</small>/In<small>₂</small>S<small>₃</small>/PdS (Pt/TO/IS/PdS) was successfully built by the step-by-step decoration of Pt and PdS nanoparticles (NPs) on the inner and outer shells of a hierarchical hollow TiO<small>₂</small>/In<small>₂</small>S<small>₃</small> (TO/IS) heterojunction, respectively. Experimental results demonstrate that the spatial separation of reduction and oxidation co-catalysts accelerates the surface redox reaction and, more importantly, promotes photo-induced charges to flow in opposite directions. By combining the virtues of TiO<small>₂</small>/In<small>₂</small>S<small>₃</small> heterojunction shell, spatially separated dual co-catalyst and extended light absorption, the Pt/TO/IS/PdS catalyst exhibits a remarkable photocatalytic H<small>₂</small> production performance under visible light irradiation, which is 36.0 times enhancement than that of the TiO<small>₂</small>/In<small>₂</small>S<small>₃</small> heterojunction. This study demonstrates that the strategy of combining heterojunctions and spatially separated co-catalysts has great reference significance for developing a highly efficient photocatalytic system.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 18","pages":" 5449-5455"},"PeriodicalIF":5.0,"publicationDate":"2023-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"7164188","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":"g-C3N4 coupled with 2,4,6-tris(4-aminophenyl)-1,3,5-triazine via π–π interactions enhanced visible-light photocatalytic H2 evolution from water splitting†","authors":"Chen-Chuang Li, Ikram Ullah, Gang Wang and An-Wu Xu","doi":"10.1039/D3CY00837A","DOIUrl":"https://doi.org/10.1039/D3CY00837A","url":null,"abstract":"<p >Graphitic carbon nitride (g-C<small>₃</small>N<small>₄</small>) is an attractive candidate among the most promising metal-free photocatalysts under visible light for solar-to-fuel production. Nevertheless, the low photocatalytic performance and fast recombination rate of photoinduced charge carriers prevent its practical applications. Therefore, the integration of g-C<small>₃</small>N<small>₄</small> with an appropriate material is highly desirable for enhancing H<small>₂</small> production. In this work, we report a TAPT/CN composite photocatalyst formed from g-C<small>₃</small>N<small>₄</small> and 2,4,6-tris(4-aminophenyl)-1,3,5-triazine (TAPT) through π–π interactions and hydrogen bonds to enhance the photocatalytic activity. The small TAPT molecules act as a hole relay and thus elevate the transfer rate of holes from g-C<small>₃</small>N<small>₄</small> to triethanolamine (TEOA); this in turn favors more electron transfer to the Pt cocatalyst and finally promotes the visible-light-driven H<small>₂</small> generation. The experimental results display that photocatalytic activity is greatly boosted by TAPT molecules in TAPT/CN nanoheterostructures. The optimized 5% TAPT/CN (5 wt% TAPT loading) sample achieves a maximum H<small>₂</small> evolution rate of 99.54 μmol h<small>⁻¹</small>, which is 7.1 times higher than that of bare g-C<small>₃</small>N<small>₄</small> (14.01 μmol h<small>⁻¹</small>). Additionally, there is no significant decrease in H<small>₂</small> production after five consecutive cycles of continuous visible-light irradiation of up to 20 hours. We expect that this research will open the door to designing other organic material-decorated g-C<small>₃</small>N<small>₄</small> photocatalysts for potential applications in solar-to-hydrogen energy conversion.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 18","pages":" 5456-5461"},"PeriodicalIF":5.0,"publicationDate":"2023-08-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"7164190","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":"Theoretical study on dry reforming of methane over a Ni(111) surface under electric fields and with alkali metal additives†","authors":"Hui Jiao and Gui-Chang Wang","doi":"10.1039/D3CY00547J","DOIUrl":"https://doi.org/10.1039/D3CY00547J","url":null,"abstract":"<p >The dry reforming of methane (DRM) reaction is an effective way to convert greenhouse gases into syngas and mitigate the greenhouse effect. However, Ni-based catalysts tend to deposit carbon and reduce catalytic activity due to the high endothermic properties of the DRM reaction. Nickel catalysts promote the DRM reaction and exhibit good catalytic activity and resistance to carbon deposition by applying external electric fields. The DRM reaction on a Ni(111) surface under electric fields of +0.6, 0, and −0.6 V Å<small>⁻¹</small> and with the K additive was systematically studied by density functional theory calculation and microkinetic modeling in this work. The results showed that electric fields can adjust the adsorption strength of species. Notably, exposed negative electric fields and alkali metals can promote the adsorption strength of oxygen-containing species by increasing the electron-donating ability and thus reducing the CO<small>₂</small> activation energy. The path of CH–O oxidation on all Ni-based catalysts was the most favorable in the DRM reaction, and the free energy span was K/Ni(111) &lt; Ni(111) (−0.6 V Å<small>⁻¹</small>) &lt; Ni(111) (+0.6 V Å<small>⁻¹</small>) &lt; Ni(111), indicating that the applied electric field (or alkali metal) is conducive to the elimination of surface carbon species. The effect of alkali metals to improve the activity and resistance to carbon deposition of Ni-based catalysts by promoting CO<small>₂</small> dissociation can be quantitatively reproduced by external negative electric fields. The degree of rate control analysis showed that the activation of CH<small>₄</small> and CO<small>₂</small> had a crucial impact on the formation rate and carbon deposition of the DRM reaction. Microkinetic modeling results showed that conversions of CH<small>₄</small> and CO<small>₂</small> were increased under a positive electric field. The carbon deposition resistance was in the order of Ni(111) (+0.6 V Å<small>⁻¹</small>) &lt; Ni(111) &lt; Ni(111) (−0.6 V Å<small>⁻¹</small>) &lt; K/Ni(111). Moreover, the H<small>₂</small>/CO ratio was smaller than the unit under a negative electric field and an alkali additive due to the facile dissociation of CO<small>₂</small>, whereas it was close to the unit under a positive electric field. Our theoretical results correspond well with experimental observations that the application of electric fields and the K additive can not only improve the catalytic activity of Ni-based catalysts but also enhance the carbon deposition resistance. This work provided an understanding of how the electric field and K additive can help eliminate carbon deposition at the atomic level.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 18","pages":" 5407-5421"},"PeriodicalIF":5.0,"publicationDate":"2023-08-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"7164185","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":"Study on the catalytic activity and hydrothermal stability of one-pot synthesized Fe-based FER zeolites for NH3-SCR†","authors":"Xinyue Hu, Jialing Chen, Shaokang He, Tingyu Liang, Shenke Zheng, Lijun Lu, Chenxi Hao, Kaixin Chen, Tingting Li, Lan Yi, Li Guo and Xiaoqin Wu","doi":"10.1039/D3CY00761H","DOIUrl":"https://doi.org/10.1039/D3CY00761H","url":null,"abstract":"<p >Three OP-Fe-FER-<em>x</em> zeolites (with an FER structure) synthesized by a one-pot method with different Si/Al ratios (<em>x</em> = Si/Al =10–30) and similar iron contents (5.4–5.6 wt%) were compared with commercial IM-Fe/SSZ-20 zeolite (with a CHA structure) prepared by an incipient wetness impregnation method to investigate their catalytic activity and hydrothermal stability for the selective catalytic reduction reaction of NO<small>_<em>x</em></small> with NH<small>₃</small> (NH<small>₃</small>-SCR). For both fresh (without hydrothermal aging treatments) and aged (with hydrothermal aging treatments) zeolites, the NO<small>_<em>x</em></small> conversions of OP-Fe-FER-<em>x</em> zeolites are much higher than that of IM-Fe/SSZ-20 zeolite, suggesting that the OP-Fe-FER-<em>x</em> zeolites are better catalysts for NH<small>₃</small>-SCR than the commercial IM-Fe/SSZ-20 zeolite. Compared with the fresh zeolites, the NO<small>_<em>x</em></small> conversions of all four aged zeolites decrease in the low-temperature range (100–300 °C), while they increase at high temperatures (450–550 °C) to different extents. Based on XRD, N<small>₂</small> physisorption, NH<small>₃</small>-TPD, UV-vis, XPS and H<small>₂</small>-TPR experiments, the hydrothermal aging process of the OP-Fe-FER-<em>x</em> zeolites is depicted, which consists of partial collapse of the zeolite framework, removal of framework aluminum and iron atoms, and transformation and aggregation of iron species. Detailed characterization reveals that the OP-Fe-FER-<em>x</em> zeolites are more stable than the IM-Fe/SSZ-20 zeolite during the hydrothermal aging treatments. The obvious decline of NH<small>₃</small>-SCR catalytic activity for the aged zeolites in the low-temperature range is mainly attributed to the transformation and aggregation behaviors of active isolated Fe<small>³⁺</small> species. As for the increase of NH<small>₃</small>-SCR activity for the aged zeolites at the high temperatures (450–550 °C), it is mainly attributed to the suppression of the NH<small>₃</small> oxidation side reaction due to the deteriorated NH<small>₃</small> storage capacity because of the loss of massive acid sites during the hydrothermal aging treatments.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 18","pages":" 5435-5448"},"PeriodicalIF":5.0,"publicationDate":"2023-08-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"7164187","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":"Cyclometalated C^N diphosphine ruthenium catalysts for Oppenauer-type oxidation/transfer hydrogenation reactions and cytotoxic activity†","authors":"Dario Alessi, Pierfrancesco Del Mestre, Eleonora Aneggi, Maurizio Ballico, Antonio P. Beltrami, Marta Busato, Daniela Cesselli, Alexandra A. Heidecker, Daniele Zuccaccia and Walter Baratta","doi":"10.1039/D3CY00676J","DOIUrl":"https://doi.org/10.1039/D3CY00676J","url":null,"abstract":"<p >The cyclometalated acetate ruthenium complexes [Ru(C^N)(η<small>²</small>-OAc)(dppb)] (dppb = 1,4-bis(diphenylphosphino)butane; HC^N = 2-phenylpyridine <strong>1</strong>, benzo[<em>h</em>]quinoline <strong>2</strong>, 1-phenylpyrazole <strong>3</strong>, 2-phenyl-2-oxazoline <strong>4</strong>) are easily obtained in 58–74% yield through a one-pot synthesis from [Ru(η<small>²</small>-OAc)<small>₂</small>(dppb)] and the corresponding phenyl substituted N-heterocycle in methanol <em>via</em> elimination of HOAc. These complexes have been characterized by single crystal X-ray diffraction studies. Protonation of <strong>2</strong> with HCO<small>₂</small>H (5 equiv.) in toluene affords the formate [Ru(C^N)(η<small>²</small>-HCO<small>₂</small>)(dppb)] (<strong>5</strong>) isolated in 75% yield, without release of the HC^N ligand. The derivatives <strong>1–4</strong> display catalytic activity in the Oppenauer-type oxidation of secondary alcohols to ketones at S/C = 1000, using acetone or cyclohexanone as hydrogen acceptor and KO<em>t</em>Bu as base in toluene, with TOF up to 12 000 h<small>⁻¹</small> for <strong>4</strong>. Complexes <strong>1–4</strong> at S/C = 1000 are also active in the TH of carbonyl compounds to alcohols in 2-propanol employing NaO<em>i</em>Pr, with TOF up to 14 300 h<small>⁻¹</small> for <strong>4</strong>. The evaluation of the cytotoxic activity of these complexes against U87 glioblastoma cancer cell line <em>via</em> MTT test affords IC<small>₅₀</small> values ranging from 1.4 to 4.1 μM.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 18","pages":" 5267-5279"},"PeriodicalIF":5.0,"publicationDate":"2023-08-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2023/cy/d3cy00676j?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"7164148","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":"CoP nanoparticles embedded in three-dimensional porous network-like structured N, O co-doped carbon nanofibers as an effective bi-functional electrocatalyst for rechargeable zinc–air batteries†","authors":"Nanping Deng ,&nbsp;Qiang Zeng ,&nbsp;Yang Feng ,&nbsp;Hongjing Gao ,&nbsp;Gang Wang ,&nbsp;Jing Yan ,&nbsp;Tinglu Zheng ,&nbsp;Yong Liu ,&nbsp;Weimin Kang ,&nbsp;Bowen Cheng","doi":"10.1039/d3cy00708a","DOIUrl":"10.1039/d3cy00708a","url":null,"abstract":"<div><p>The development of noble metal-free bi-functional electrocatalysts is consistent with the current concept of sustainable development of energy systems. In this study, we develop a strategy to prepare ZIF-67-derived CoP nanoparticles embedded in three-dimensional porous network-like structured N, O co-doped carbon nanofibers (CoP@N, O co-doped PCNFs) through the processes of electro-blown spinning, carbonization, and <em>in situ</em> phosphorization. And they are regarded as an ORR/OER bi-functional electrocatalyst, which is applied in rechargeable zinc–air batteries. The hierarchically porous structure of the carbon nanofibers facilitates the diffusion of dissolved oxygen and the formation of abundant gas–liquid–solid interfaces in the liquid electrolyte, leading to enhanced ORR/OER activity. Therefore, the ORR half-wave potential of the CoP@N, O co-doped PCNFs reached 0.81 V. In particular, the OER overpotential exhibited 250 mV at 10 mA cm⁻². More importantly, the zinc–air battery constructed with the CoP@N, O co-doped PCNF catalyst has a high specific capacity (797.2 mA h g⁻¹) and energy density (927.9 W h kg⁻¹) at a current density of 10 mA cm⁻² and can stably cycle for 500 h at a current density of 2 mA cm⁻². The findings will provide a new paradigm for designing more practical noble metal-free bi-functional electrocatalysts for rechargeable zinc–air batteries.</p></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"13 16","pages":"Pages 4823-4838"},"PeriodicalIF":5.0,"publicationDate":"2023-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"3949949","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":"Role of polyoxometalate precursors and supports in the selective oxidation of methane into formaldehyde using supported metal oxide subnanocluster catalysts†","authors":"Keiju Wachi ,&nbsp;Tomohiro Yabe ,&nbsp;Takaaki Suzuki ,&nbsp;Kentaro Yonesato ,&nbsp;Kosuke Suzuki ,&nbsp;Kazuya Yamaguchi","doi":"10.1039/d3cy00750b","DOIUrl":"10.1039/d3cy00750b","url":null,"abstract":"<div><p>The direct synthesis of useful chemicals from methane (CH₄) is desirable; however, the products are prone to nonselective overoxidation, leading to the formation of CO₂. A previous study developed a supported iron oxide subnanocluster catalyst with high thermal stability using iron-containing polyoxometalates (POMs) as precursors to selectively produce formaldehyde (HCHO) and CO. Herein, we investigated various supported POM-based catalysts to further improve the selectivity to HCHO <em>via</em> CH₄ oxidation, specifically by suppressing the pyrolysis and overoxidation of HCHO. After examining various metal-containing POM precursors and supports, we found that catalysts prepared using mononuclear- and dinuclear-iron-containing POM precursors supported on SiO₂ with a high specific surface area were effective and yielded relatively high quantities of HCHO. <em>In situ</em> diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) measurements under HCHO flow demonstrated that the pyrolysis and oxidation of HCHO were suppressed on SiO₂, while the pyrolysis of HCHO was promoted on Al₂O₃. Furthermore, <em>in situ</em> DRIFTS measurements conducted at different temperatures revealed that HCHO was not decomposed or oxidized at 500 °C in the absence of catalysts.</p></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"13 16","pages":"Pages 4744-4752"},"PeriodicalIF":5.0,"publicationDate":"2023-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"3965224","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":"Enhancing solar-to-hydrogen efficiency with an S-scheme GaTe/PtS2 van der Waals heterojunction with high light absorption†","authors":"Jiaxin Wang ,&nbsp;Jinzhe Xuan ,&nbsp;Xing Wei ,&nbsp;Yan Zhang ,&nbsp;Jibin Fan ,&nbsp;Lei Ni ,&nbsp;Yun Yang ,&nbsp;Jian Liu ,&nbsp;Ye Tian ,&nbsp;Xuqiang Wang ,&nbsp;Chongrong Yuan ,&nbsp;Li Duan","doi":"10.1039/d3cy00610g","DOIUrl":"10.1039/d3cy00610g","url":null,"abstract":"<div><p>To tackle the urgent challenges posed by the current energy crisis and environmental concerns, the potential of photocatalytic water splitting has been recognized as a promising solution. In this study, we investigate the structural, electronic, and optical properties of a van der Waals heterojunction (vdwH) formed by combining GaTe and PtS₂ using first-principles calculations. We also examine the Bader charge and solar hydrogen efficiency of this heterojunction to gain insights into its potential for practical applications. The GaTe/PtS₂ heterojunction as a step-scheme (S-scheme) heterojunction has a similar structure to the traditional type-II heterojunction, that is, photo-generated carriers can be automatically separated in space. Analysis of the average charge density difference reveals the presence of a built-in electric field within the heterojunction, which effectively extends the lifetime of carriers. When pH = 0, GaTe/PtS₂ can promote a redox reaction to split water. The high photocatalytic activity of GaTe/PtS₂ is evidenced by its strong light absorption coefficient in the absorption spectrum. Effective modification of the band edge position and optical properties can be achieved through biaxial strain, resulting in increased participation of photons in water splitting. Additionally, the GaTe/PtS₂ heterojunction boasts an impressive solar-to-hydrogen efficiency of 45.88%, and when <em>ε</em> = 4%, the <em>η</em>_STH reaches 52.18%. Thus, our study demonstrates that the GaTe/PtS₂ heterojunction is a promising S-scheme photocatalyst for comprehensive water splitting.</p></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"13 16","pages":"Pages 4753-4764"},"PeriodicalIF":5.0,"publicationDate":"2023-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"3965225","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}