Chinese Journal of Catalysis最新文献

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Platinum clusters stabilized by zincosilicate zeolite for efficient propane dehydrogenation 用硅酸锌沸石稳定铂团簇用于丙烷的高效脱氢
IF 15.7 1区 化学
Chinese Journal of Catalysis Pub Date : 2025-04-01 DOI: 10.1016/S1872-2067(24)60258-5
Hao Liu , Ying Zhang , Liyang Liu , Tianxiang Chen , Xingcong Zhang , Peng Hu , Chao Xiong , Jie Zhou , Hao Zhang , Lihui Dong , Tsz Woon Benedict Lo , Bing Nan , Xiaohui He , Hongbing Ji
{"title":"Platinum clusters stabilized by zincosilicate zeolite for efficient propane dehydrogenation","authors":"Hao Liu ,&nbsp;Ying Zhang ,&nbsp;Liyang Liu ,&nbsp;Tianxiang Chen ,&nbsp;Xingcong Zhang ,&nbsp;Peng Hu ,&nbsp;Chao Xiong ,&nbsp;Jie Zhou ,&nbsp;Hao Zhang ,&nbsp;Lihui Dong ,&nbsp;Tsz Woon Benedict Lo ,&nbsp;Bing Nan ,&nbsp;Xiaohui He ,&nbsp;Hongbing Ji","doi":"10.1016/S1872-2067(24)60258-5","DOIUrl":"10.1016/S1872-2067(24)60258-5","url":null,"abstract":"<div><div>Dispersing metals from nanoparticles to clusters is often achieved using ligand protection methods, which exhibit unique properties such as suppressing structure-sensitive side reactions. However, this method is limited by the use of different metal precursor salts corresponding to different ligands. An alternative approach, the ion exchange (IE) method, can overcome this limitation to some extent. Nevertheless, there is still an urgent need to address the stabilization of metals (especially precious metals) by using IE method. Here, we reported a Pt cluster catalyst prepared mainly by anchoring Pt atoms via O located near the framework Zn in zincosilicate zeolites and riveted by zeolite surface rings after reduction (reduced Pt/Zn-3-IE). The catalyst can achieve an initial propane conversion of 26% in a pure propane atmosphere at 550 °C and shows little deactivation even after 7.5 d of operation. Moreover, the alteration of catalyst by the introduction of framework Zn was also highlighted and interpreted.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"71 ","pages":"Pages 208-219"},"PeriodicalIF":15.7,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143860197","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Chelating-agent-free incorporation of isolated Ni single-atoms within BEA zeolite for enhanced biomass hydrogenation 在BEA沸石中无螯合剂掺入分离的Ni单原子以增强生物质加氢
IF 15.7 1区 化学
Chinese Journal of Catalysis Pub Date : 2025-04-01 DOI: 10.1016/S1872-2067(24)60272-X
Meng Liu , Caixia Miao , Yumeng Fo , Wenxuan Wang , Yao Ning , Shengqi Chu , Weiyu Song , Ying Zhang , Jian Liu , Zhijie Wu , Wenhao Luo
{"title":"Chelating-agent-free incorporation of isolated Ni single-atoms within BEA zeolite for enhanced biomass hydrogenation","authors":"Meng Liu ,&nbsp;Caixia Miao ,&nbsp;Yumeng Fo ,&nbsp;Wenxuan Wang ,&nbsp;Yao Ning ,&nbsp;Shengqi Chu ,&nbsp;Weiyu Song ,&nbsp;Ying Zhang ,&nbsp;Jian Liu ,&nbsp;Zhijie Wu ,&nbsp;Wenhao Luo","doi":"10.1016/S1872-2067(24)60272-X","DOIUrl":"10.1016/S1872-2067(24)60272-X","url":null,"abstract":"<div><div>Precisely tailoring metal single-atoms within zeolite scattfolds and understanding the origin of the unique behavior of such atomically dispersed catalysts are pivotal and challenge in chemistry and catalysis. Herein, we have successfully fabricated Ni single-atoms within BEA zeolite (Ni<sub>1</sub>@Beta) through a facile <em>in situ</em> two-step hydrothermal strategy, notably without using any chelating agent for stabilizing Ni species. With the aid of advanced characterization techniques, such as aberration-corrected high-angle annular dark-field scanning transmission electron microscopy, X-ray absorption spectroscopy, etc., and combined with density functional theory calculations, the nature and micro-environment of isolated Ni species, which are incorporated within 6-membered rings and stabilized by four skeletal oxygens of Beta zeolite, have been identified. The as-obtained Ni<sub>1</sub>@Beta exhibits a superior performance in terms of activity (with a turnover frequency value up to 114.1 h<sup>–1</sup>) and stability (for 5 consecutive runs) in the selective hydrogenation of furfural, surpassing those of Ni nanoparticle analogues and previously reported Ni-based heterogeneous catalysts. This study provides an efficient strategy for the fabrication of non-noble metal single-atoms within zeolites, which could be of great help for the design of metal-zeolite combinations in the chemoselective reactions involved in biomass conversion and beyond.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"71 ","pages":"Pages 308-318"},"PeriodicalIF":15.7,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143860201","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Synthesis of 5-hydroxymethylfurfural and its oxidation derivatives by immobilized catalysts: An efficient green sustainable technology 利用固定化催化剂合成 5-羟甲基糠醛及其氧化衍生物:一种高效的绿色可持续技术
IF 15.7 1区 化学
Chinese Journal of Catalysis Pub Date : 2025-04-01 DOI: 10.1016/S1872-2067(24)60274-3
Yao Chen , Jun Ge
{"title":"Synthesis of 5-hydroxymethylfurfural and its oxidation derivatives by immobilized catalysts: An efficient green sustainable technology","authors":"Yao Chen ,&nbsp;Jun Ge","doi":"10.1016/S1872-2067(24)60274-3","DOIUrl":"10.1016/S1872-2067(24)60274-3","url":null,"abstract":"<div><div>5-Hydroxymethylfurfural (HMF) and its oxidation derivatives have emerged as a bridge between biomass resources and the future energy industry. These renewable biomass resources can be transformed into a variety of value-added chemicals, thereby addressing the challenges posed by diminishing fossil fuel reserves and environmental concerns. The immobilization of catalysts represents an innovative method for the sustainable and efficient synthesis of HMF and its oxidation derivatives. This method not only enhances the yield and selectivity of the products but also allows for the optimization of the catalytic performance of immobilized catalysts through the strategic design of their supports. In this review, we provide an overview of the recent advancements in the technology of immobilized catalyst and its application in the synthesis of HMF and its oxidation derivatives, with a particular focus on the preparation and catalytic characteristics of these immobilized catalysts. Furthermore, we discuss potential future directions for the development of immobilized catalysts, including the preparation of high-performance immobilized catalysts, the exploration of their growth and catalytic mechanisms, and the economic implications of raw material utilization. This area of research presents both significant promise and considerable challenges.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"71 ","pages":"Pages 5-24"},"PeriodicalIF":15.7,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143859521","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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 role of C1 species in the methanol-to-hydrocarbons reaction: Beyond merely being reactants C1在甲醇制烃反应中的作用:不仅仅是作为反应物
IF 15.7 1区 化学
Chinese Journal of Catalysis Pub Date : 2025-04-01 DOI: 10.1016/S1872-2067(24)60228-7
Yanan Zhang , Wenna Zhang , Chengwei Zhang , Linhai He , Shanfan Lin , Shutao Xu , Yingxu Wei , Zhongmin Liu
{"title":"The role of C1 species in the methanol-to-hydrocarbons reaction: Beyond merely being reactants","authors":"Yanan Zhang ,&nbsp;Wenna Zhang ,&nbsp;Chengwei Zhang ,&nbsp;Linhai He ,&nbsp;Shanfan Lin ,&nbsp;Shutao Xu ,&nbsp;Yingxu Wei ,&nbsp;Zhongmin Liu","doi":"10.1016/S1872-2067(24)60228-7","DOIUrl":"10.1016/S1872-2067(24)60228-7","url":null,"abstract":"<div><div>In the methanol-to-hydrocarbons (MTH) process, C1 species, including methanol, dimethyl ether, and surface methoxy species (SMS), play crucial roles in the evolution of organic species and the construction of reaction networks. Understanding the roles of C1 species throughout the entire MTH process is both essential and challenging. Herein, the dynamic evolution of organic species and unique variation of C1 species during the real-time MTH process were observed by <em>operando</em> diffused reflectance Fourier transform infrared spectroscopy and <em>ex-situ</em> <sup>13</sup>C cross polarization/magic-angle spinning nuclear magnetic resonance experiments. Importantly, density functional theory calculations thoroughly illustrated that methanol and SMS serve as key C1 species, in the form of not only methylation agents but also hydride acceptors, and their contributions vary across different reaction periods. Initially, SMS acts as the preferential C1 surface intermediate, methylating with hydrocarbons to propagate C–C bond, while also accepting hydrides to generate precursors for active hydrocarbon pool species. As reaction progresses, the role of SMS gradually diminishes, and thereby methanol becomes the predominant C1 species, in methylation for efficient product formation, meanwhile in hydride-transfer causing catalyst deactivation. Additionally, it was demonstrated that the confined zeolite microenvironment modified by large organics affects methanol adsorption and SMS formation, also accounting for the absence of SMS during the later period of reaction. This work provides a comprehensive and systematic understanding of the dynamic roles of C1 species throughout the MTH process, beyond the role as reactants.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"71 ","pages":"Pages 169-178"},"PeriodicalIF":15.7,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143859529","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Highly dispersed MoOx-Ru/C bimetallic catalyst for efficient hydrogenolysis of esters to alkanes 高分散MoOx-Ru/C双金属催化剂,用于酯类高效氢解制烷烃
IF 15.7 1区 化学
Chinese Journal of Catalysis Pub Date : 2025-04-01 DOI: 10.1016/S1872-2067(24)60254-8
Xincheng Cao , Jiaping Zhao , Feng Long , Peng Liu , Yuguo Dong , Zupeng Chen , Junming Xu , Jianchun Jiang
{"title":"Highly dispersed MoOx-Ru/C bimetallic catalyst for efficient hydrogenolysis of esters to alkanes","authors":"Xincheng Cao ,&nbsp;Jiaping Zhao ,&nbsp;Feng Long ,&nbsp;Peng Liu ,&nbsp;Yuguo Dong ,&nbsp;Zupeng Chen ,&nbsp;Junming Xu ,&nbsp;Jianchun Jiang","doi":"10.1016/S1872-2067(24)60254-8","DOIUrl":"10.1016/S1872-2067(24)60254-8","url":null,"abstract":"<div><div>The efficient hydrogenolysis of esters to alkanes is the key protocol for producing advanced biofuels from renewable plant oils or fats. Due to the low reactivity of the carbonyl group in esters, a high reaction temperature (&gt;250 °C) is the prerequisite to ensure high conversion of esters. Here, we report a highly dispersed MoO<sub><em>x</em></sub>-Ru/C bimetallic catalyst for the efficient hydrogenolysis of esters to alkanes under 150 °C. The optimal catalyst exhibits &gt;99% conversion of methyl stearate and 99% selectivity to diesel-range alkanes, reaching a high rate of up to 2.0 mmol g<sub>cat</sub><sup>–1</sup> h<sup>–1</sup>, 5 times higher than that of Ru/C catalyst (MoO<sub><em>x</em></sub>/C is inert). Integrated experimental and theoretical investigations attribute the high performance to the abundant MoO<sub><em>x</em></sub>-Ru interfacial sites on the catalyst surface, which offers high activity for the C–O cleavage of esters. Furthermore, the dispersed MoO<sub><em>x</em></sub> species significantly weaken the hydrocracking activity of the metallic Ru for C–C bonds, thus yielding alkane products without carbon loss. This study provides a facile and novel strategy for the design of high-performance heterogeneous catalysts for the hydrodeoxygenation of biomass-derived esters to alkane products.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"71 ","pages":"Pages 256-266"},"PeriodicalIF":15.7,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143860095","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
All solid-solution S-scheme heterojunction with adjustable internal electric field for highly efficient photocatalytic activity 全固溶s型异质结,具有可调的内部电场,具有高效的光催化活性
IF 15.7 1区 化学
Chinese Journal of Catalysis Pub Date : 2025-04-01 DOI: 10.1016/S1872-2067(24)60275-5
Shiya Yue , Rong Li , Zhengrong Wei , Yun Gao , Karen Wilson , Xuxing Chen
{"title":"All solid-solution S-scheme heterojunction with adjustable internal electric field for highly efficient photocatalytic activity","authors":"Shiya Yue ,&nbsp;Rong Li ,&nbsp;Zhengrong Wei ,&nbsp;Yun Gao ,&nbsp;Karen Wilson ,&nbsp;Xuxing Chen","doi":"10.1016/S1872-2067(24)60275-5","DOIUrl":"10.1016/S1872-2067(24)60275-5","url":null,"abstract":"<div><div>Developing an efficient photocatalyst is the key to realize the practical application of photocatalysis. The S-scheme heterojunction has great potential in photocatalysis due to its unique charge-carrier migration pathway, effective light absorption and high redox capacity. However, further enhancing the built-in electric field of the S-scheme, accelerating carrier separation, and achieving higher photocatalytic performance remain unresolved challenges. Herein, based on the continuously adjustable band structure of continuous solid-solution, a novel 0D/2D all solid-solution S-scheme heterojunction with adjustable internal electric field was designed and fabricated by employing a solid-solution of Zn<sub><em>x</em></sub>Cd<sub>1–<em>x</em></sub>S and Bi<sub>2</sub>Mo<sub><em>y</em></sub>W<sub>1–<em>y</em></sub>O<sub>6</sub> respectively as reduction and oxidation semiconductors. The synergistic optimization of effective light absorption, fast photogenerated carrier separation, and high redox potential leads can be tuned to promote photocatalytic activity. Under visible light, the S-scheme system constructed by Zn<sub>0.4</sub>Cd<sub>0.6</sub>S quantum dot (QDs) and Bi<sub>2</sub>Mo<sub>0.2</sub>W<sub>0.8</sub>O<sub>6</sub> monolayer exhibits a high rate for photocatalytic degradation C<sub>2</sub>H<sub>4</sub> (150.6 × 10<sup>–3</sup> min<sup>–1</sup>), which is 16.5 times higher than that of pure Zn<sub>0.4</sub>Cd<sub>0.6</sub>S (9.1 × 10<sup>–3</sup> min<sup>–1</sup>) and 53.8 times higher than pure Bi<sub>2</sub>Mo<sub>0.2</sub>W<sub>0.8</sub>O<sub>6</sub> (2.8 × 10<sup>–3</sup> min<sup>–1</sup>). Due to the unique charge-carrier migration pathway, photo-corrosion of Zn<sub><em>x</em></sub>Cd<sub>1–<em>x</em></sub>S is further inhibited simultaneously. <em>In-situ</em> irradiation X-ray photoelectron spectroscopy, photoluminescence spectroscopy, time-resolved photoluminescence, transient absorption spectroscopy and electron paramagnetic resonance provide compelling evidence for interfacial charge transfer <em>via</em> S-scheme pathways, while <em>in-situ</em> diffuse reflectance infrared Fourier transform spectroscopy identifies the reaction pathway for C<sub>2</sub>H<sub>4</sub> degradation. This novel S-scheme photocatalysts demonstrates excellent performance and potential for the practical application of the fruits and vegetables preservation at room temperatures.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"71 ","pages":"Pages 353-362"},"PeriodicalIF":15.7,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143860205","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Zeolites in the epoch of catalytic recycling plastic waste: Toward circular economy and sustainability 催化回收塑料废物时代的沸石:走向循环经济和可持续性
IF 15.7 1区 化学
Chinese Journal of Catalysis Pub Date : 2025-04-01 DOI: 10.1016/S1872-2067(24)60273-1
Qing Liu , Jin Shang , Zhendong Liu
{"title":"Zeolites in the epoch of catalytic recycling plastic waste: Toward circular economy and sustainability","authors":"Qing Liu ,&nbsp;Jin Shang ,&nbsp;Zhendong Liu","doi":"10.1016/S1872-2067(24)60273-1","DOIUrl":"10.1016/S1872-2067(24)60273-1","url":null,"abstract":"<div><div>Current ever-accumulating plastic waste can be considered a significant carbon resource for energy conversion and chemical production. The development of new approaches for upcycling plastic waste through chemical degradation may enable circularity and promote closed-loop recycling of carbon sources compared to traditional recycling methods. Zeolite, a widely used solid acid catalyst with high industrial potential in petroleum and biomass refining, has been extensively studied for its role in transforming plastics. In this review, we present an overview of zeolite-based catalytic systems for the chemical recycling of plastic waste and discuss how zeolites could potentially contribute to the future development of a circular economy. To provide a comprehensive understanding, we begin with a brief introduction to zeolites, analyzing their key features and exploring their opportunities as well as challenges in processing plastic waste. Subsequently, we delve into the chemistry of catalytic cracking and tandem catalysis using zeolite-based catalysts on plastics. Overall, we emphasize the importance of intelligent catalyst design and lower-energy pathways to incentivize plastic upcycling while alleviating the burden caused by waste plastics.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"71 ","pages":"Pages 54-69"},"PeriodicalIF":15.7,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143859523","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Advances in humins formation mechanism, inhibition strategies, and value-added applications 腐植酸形成机理、抑制策略和增值应用方面的进展
IF 15.7 1区 化学
Chinese Journal of Catalysis Pub Date : 2025-04-01 DOI: 10.1016/S1872-2067(24)60248-2
Yitong Wang , Chaofeng Zhang , Cheng Cai , Caoxing Huang , Xiaojun Shen , Hongming Lou , Changwei Hu , Xuejun Pan , Feng Wang , Jun Xie
{"title":"Advances in humins formation mechanism, inhibition strategies, and value-added applications","authors":"Yitong Wang ,&nbsp;Chaofeng Zhang ,&nbsp;Cheng Cai ,&nbsp;Caoxing Huang ,&nbsp;Xiaojun Shen ,&nbsp;Hongming Lou ,&nbsp;Changwei Hu ,&nbsp;Xuejun Pan ,&nbsp;Feng Wang ,&nbsp;Jun Xie","doi":"10.1016/S1872-2067(24)60248-2","DOIUrl":"10.1016/S1872-2067(24)60248-2","url":null,"abstract":"<div><div>Humins, as a group of by-products formed through the condensation and coupling of fragment intermediates during lignocellulosic biomass refining, can cause numerous negative effects such as the wastage of carbon resources, clogging of reactor piping, deactivation of catalyst, and barriers to product separation. Elucidating the generation mechanism of humins, developing efficient inhibitors, and even utilizing them as a resource, both from the perspective of atom economy and safe production, constitutes a research endeavor replete with challenges and opportunities. Orbiting the critical issue of humins structure and its generation mechanism from cellulose and hemicellulose resources, the random condensation between intermediates such as 5-hydroxymethylfurfural, furfural, 2,5-dioxo-6-hydroxyhexanal, and 1,2,4-benzenetriol etc. were systematically summarized. Additionally, the presence of lignin in real biorefining processes further promotes the formation of a special type of humins known as “pseudo-lignin”. The influences of various factors, including raw materials, reaction temperature and time, acid-base environment, as well as solvent systems and catalysts, on the formation of humins were comprehensively analyzed. To minimize the formation of humins, the design of efficient solvent systems and catalysts is crucial. Furthermore, this review investigates the approaches to value-added applications of humins. The corresponding summary could provide guidance for the development of the humins chemistry.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"71 ","pages":"Pages 25-53"},"PeriodicalIF":15.7,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143859522","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Designed electron transport path via Fe–O–Ni atomic bond for high CO2 reduction 设计了通过Fe-O-Ni原子键的电子传递路径,用于高CO2还原
IF 15.7 1区 化学
Chinese Journal of Catalysis Pub Date : 2025-04-01 DOI: 10.1016/S1872-2067(24)60230-5
Mengyang Xu , Bingqing Chang , Jinze Li , Huiqin Wang , Pengwei Huo
{"title":"Designed electron transport path via Fe–O–Ni atomic bond for high CO2 reduction","authors":"Mengyang Xu ,&nbsp;Bingqing Chang ,&nbsp;Jinze Li ,&nbsp;Huiqin Wang ,&nbsp;Pengwei Huo","doi":"10.1016/S1872-2067(24)60230-5","DOIUrl":"10.1016/S1872-2067(24)60230-5","url":null,"abstract":"<div><div>The assembly of different Metal organic framework (MOFs) into hybrid heterostructures has proven to be a promising strategy that can effectively break through the limited regulatory capacity of single metal sites. Here, an S-scheme heterostructure (Fe<sub>3</sub>Ni-MOF) based on homologous ligands (1,4-phthalic acid) of ultra-thin Ni-MOF and Fe-MOF nanoparticles with directional electron transport channels, was developed and used it for photoreduction of CO<sub>2</sub>. Under the S-scheme electric field mechanism, the photogenerated carrier can achieve efficient directional separation through Fe–O–Ni atomic bond, which significantly reduces the energy barrier of the rate-determining step. Results show that the performance of Fe<sub>3</sub>Ni-MOF (63.5 μmol g<sup>–1</sup>) was 20 and 3.2 times higher than that of Ni-MOF and Fe-MOF, respectively, and exhibits excellent CO selectivity (96.4%) and stability. Transmission electron microscopy and atomic force microscopy revealed the two-molecular-layers structure of Ni-MOF and the micro-assembly structure of Fe<sub>3</sub>Ni-MOF, which can shorten the electron transport distance and increase the molecular mass transfer rate. X-ray photoelectron spectroscopy, electron spin resonance and electron density difference calculations reveal that interfacial electric fields and atomic bonds work together to promote directional carrier separation, resulting in the accumulation of holes on Ni-MOF and electrons on Fe-MOF. The Gibbs free energy calculation and <em>in-situ</em> Fourier transformed infrared spectroscopy validate that the micro-assembled S-scheme heterostructures with directional electron transport channels can significantly reduce the activation energy barrier of the reaction. This study not only proves the feasibility of constructing MOFs S-scheme heterostructures using homologous ligands, but also provides a new way to overcome the limitations of monometallic MOFs. This strategy is expected to open up a new avenue to design efficient photocatalysts.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"71 ","pages":"Pages 114-127"},"PeriodicalIF":15.7,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143860096","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Insights into Structure-Activity Relationships between Y Zeolites and their n-C10 Hydrocracking Performances via Machine Learning Approaches 利用机器学习方法研究Y型沸石及其n-C10加氢裂化性能的构效关系
IF 15.7 1区 化学
Chinese Journal of Catalysis Pub Date : 2025-04-01 DOI: 10.1016/S1872-2067(24)60259-7
Qianli Ma , Hong Nie , Ping Yang , Jianqiang Liu , Hongyi Gao , Wei Wang , Songtao Dong
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