EES catalysis最新文献

{"title":"Selective glycerol to lactic acid conversion via a tandem effect between platinum and metal oxides with abundant acid groups†","authors":"Hui Luo, Mianle Xu, Sihang Liu, Giulia Tarantino, Hanzhi Ye, Hossein Yadegari, Alain Y. Li, Ceri Hammond, Georg Kastlunger, Ifan E. L. Stephens and Maria-Magdalena Titirici","doi":"10.1039/D4EY00236A","DOIUrl":"https://doi.org/10.1039/D4EY00236A","url":null,"abstract":"<p >Phasing out petrochemical-based thermoplastics with bio-plastics produced in an energy efficient and environmentally friendly way is of paramount interest. Among them, polylactic acid (PLA) is the flagship with its production accounting for 19% of the entire bioplastics industry. Glycerol electrolysis for producing the monomer lactic acid, while co-generating green H<small>₂</small>, represents a promising approach to boost the production of PLA, yet the reaction selectivity has been a bottleneck. Here, we report a combined electrochemical and chemical route using a tandem Pt/C-γ-Al<small>₂</small>O<small>₃</small> multicomponent catalyst which can achieve a glycerol-to-lactic acid selectivity of 61.3 ± 1.2%, among the highest performance reported so far. Combining an experimental and computational mechanistic analysis, we suggest that tuning the acidic sites on the catalyst surface is crucial for shifting the reaction towards the dehydration pathway, occurring <em>via</em> dihydroxyacetone intermediate. Within the tandem effect, Pt is the active site to electrochemically catalyze glycerol to dihydroxyacetone and glyceraldehyde, while the γ-Al<small>₂</small>O<small>₃</small> provides the required acidic sites for catalyzing dihydroxyacetone to the pyruvaldehyde intermediate, which will then go through Cannizzaro rearrangement, catalyzed by the OH<small>⁻</small> ions to form lactic acid. This catalytic synergy improves the selectivity towards lactic acid by nearly two-fold. A selectivity descriptor (Δ<em>G</em><small>_GLAD*</small> − Δ<em>G</em><small>_DHA*</small>) from density functional theory calculations was identified, which could be used to screen other materials in further research. Our findings highlight the promise of tandem electrolysis in the development of strategies for selective electrochemical production of high-value commodity chemicals from low value (waste) precursors.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 1","pages":" 87-96"},"PeriodicalIF":0.0,"publicationDate":"2024-11-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ey/d4ey00236a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142994073","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Self-assembled infinite silver cluster with atomic precision as a scalable catalyst for CO2-electroreduction under industry-relevant reaction rates†","authors":"Leonard Curet, William Lafargue dit-Hauret, Jordi Benet-Buchholz, Marta Martínez-Belmonte, Dominique Foix, Emilio Palomares, Laurent Billon, Didier Begué and Aurelien Viterisi","doi":"10.1039/D4EY00160E","DOIUrl":"https://doi.org/10.1039/D4EY00160E","url":null,"abstract":"<p >The multi-gram synthesis of a phenylacetylide silver cluster catalyst and its application to the electroreduction of CO<small>₂</small> to carbon monoxide is described. The procedure involves one synthetic step from commercially available precursors and yields highly crystalline silver acetylide clusters in quantitative yields with no required purification. The crystal structure of the cluster was resolved from the native powder using cutting-edge electron diffraction techniques (3D-ED), and showed to consist of an infinite silver tubular core with radially disposed phenylacetylene ligands. Its catalytic properties were investigated at industry-relevant rates in a flow cell electrolyser. Faradaic efficiencies for CO above 95% were achieved at current densities reaching 350 mA cm<small>⁻²</small>. The catalyst's selectivity and stability were shown to be the result of the unique polymeric structure, a result supported by electrochemical characterisation and DFT modelling.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 2","pages":" 286-296"},"PeriodicalIF":0.0,"publicationDate":"2024-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ey/d4ey00160e?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143564279","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Correction: High photocatalytic yield in the non-oxidative coupling of methane using a Pd–TiO2 nanomembrane gas flow-through reactor","authors":"Victor Longo, Luana De Pasquale, Francesco Tavella, Mariam Barawi, Miguel Gomez-Mendoza, Víctor de la Peña O’Shea, Claudio Ampelli, Siglinda Perathoner, Gabriele Centi and Chiara Genovese","doi":"10.1039/D4EY90022G","DOIUrl":"10.1039/D4EY90022G","url":null,"abstract":"<p >Correction for ‘High photocatalytic yield in the non-oxidative coupling of methane using a Pd–TiO<small>₂</small> nanomembrane gas flow-through reactor’ by Victor Longo <em>et al.</em>, <em>EES. Catal.</em>, 2024, <strong>2</strong>, 1164–1175, https://doi.org/10.1039/D4EY00112E.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 6","pages":" 1320-1320"},"PeriodicalIF":0.0,"publicationDate":"2024-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11475650/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142486076","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Progress in in situ characterization of electrocatalysis","authors":"Wei Shen, Yizhen Ye, Qiujin Xia and Pinxian Xi","doi":"10.1039/D4EY00168K","DOIUrl":"https://doi.org/10.1039/D4EY00168K","url":null,"abstract":"<p >With the continuous development and extensive research of electrocatalytic technology, the unclear dynamic catalytic reaction process limits the in-depth study of reaction regulation mechanisms and the targeted design of excellent catalysts. The comprehension of electrochemical reactions through conventional <em>ex situ</em> characterization techniques poses a formidable challenge. Fortunately, <em>in situ</em> characterization technology makes it possible to further clarify the mechanism of electrocatalytic reactions. Here, we will select some highlight studies of <em>in situ</em> characterization techniques during electrochemical reactions to introduce features and difficulties in practical experiments and give some advice and evaluate future development trends for relevant fields. This article will show the advantages as well as challenges in the <em>in situ</em> technology in electrocatalytic reactions, and indicate the development directions.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 1","pages":" 10-31"},"PeriodicalIF":0.0,"publicationDate":"2024-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ey/d4ey00168k?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142994105","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Interplanar synergy of a copper-based electrocatalyst favors the reduction of CO2 into C2+ products†","authors":"Jiangnan Li, Xinyi Duan, Chao Wu, Yucheng Cao, Zhiyao Duan, Wenjun Fan, Peng Zhang and Fuxiang Zhang","doi":"10.1039/D4EY00141A","DOIUrl":"https://doi.org/10.1039/D4EY00141A","url":null,"abstract":"<p >Although electrocatalytic reduction of carbon dioxide (CO<small>₂</small>) into chemicals and fuels over Cu-based catalysts has been extensively investigated, the influence of their exposed facets on product selectivity remains elusive. To address this, a series of Cu-based catalysts with different ratios of exposed Cu(100) and Cu(111) facets were synthesized and examined for CO<small>₂</small> electroreduction, based on which a remarkable interplanar synergistic effect on the selectivity of C<small>₂₊</small> products was demonstrated. The optimized Cu-based interplanar synergistic catalyst could deliver a faradaic efficiency of 78% with a C<small>₂₊</small> partial current density of 663 mA cm<small>⁻²</small>, which is extremely superior to that of its corresponding Cu counterparts with only the Cu(111) or Cu(100) facet. The interplanar synergistic effect was disclosed using density functional theory calculations to mainly benefit from favorable adsorption and activation of CO<small>₂</small> into *CO on the Cu(111) facet and significantly promoted C–C coupling on the interface of the Cu(111) and Cu(100) facets, as confirmed by observation of the favorable surface coverage of atop-bound and bridge-bound *CO as well as formation of *OC–CHO intermediates during <em>in situ</em> infrared spectroscopy analysis.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 1","pages":" 80-86"},"PeriodicalIF":0.0,"publicationDate":"2024-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ey/d4ey00141a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142994113","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"A supported Au/HZSM-5 catalyst for toluene removal by air plasma catalytic oxidation using the cycled storage-discharge (CSD) mode†","authors":"Amin Zhou, Xiao-Song Li, Jing-Lin Liu, Lan-Bo Di and Ai-Min Zhu","doi":"10.1039/D4EY00159A","DOIUrl":"https://doi.org/10.1039/D4EY00159A","url":null,"abstract":"<p >Air plasma catalytic oxidation of toluene (C<small>₇</small>H<small>₈</small>) with the cycled storage-discharge (CSD) mode is a promising technology for toluene (C<small>₇</small>H<small>₈</small>) removal. However, the problem of low CO<small>₂</small> selectivity must be solved. In this work, a novel HZSM-5 (HZ) supported Au catalyst (Au/HZ) with <em>ca.</em> 5.7 nm Au nanoparticles was prepared by combining impregnation-ammonia washing and plasma treatment, and adopted for C<small>₇</small>H<small>₈</small> removal. Au/HZ displays a large breakthrough capacity and an excellent oxidation ability of C<small>₇</small>H<small>₈</small> in dry and wet air plasma. To investigate the mechanism of CO<small>₂</small> selectivity improvement with the Au/HZ catalyst, air plasma catalytic oxidation of gaseous C<small>₇</small>H<small>₈</small> and CO, as well as the adsorption of C<small>₇</small>H<small>₈</small> and CO on the catalysts were conducted. For plasma-catalytic oxidation of gaseous C<small>₇</small>H<small>₈</small> over Au/HZ, the CO<small>₂</small> selectivity is 97.5%, significantly higher than those of HZ (55%) and Ag/HZ (62%). <em>In situ</em> TPD tests indicate that Au/HZ possesses a moderate adsorption strength for CO and C<small>₇</small>H<small>₈</small> compared with HZ and Ag/HZ. Meanwhile, plasma oxidation of CO over Au/HZ reaches 100%, which is much higher than those of HZ (15%) and Ag/HZ (24%). Nearly 100% C<small>₇</small>H<small>₈</small> conversion and CO<small>₂</small> selectivity of plasma-catalytic oxidation of C<small>₇</small>H<small>₈</small> on Au/HZ can be attributed to the moderate adsorption strength of Au/HZ for C<small>₇</small>H<small>₈</small> and CO, and very high plasma catalytic activity for CO oxidation.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 1","pages":" 97-105"},"PeriodicalIF":0.0,"publicationDate":"2024-10-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ey/d4ey00159a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142994075","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Embedding the intermetallic Pt5Ce alloy in mesopores through Pt–C coordination layer interactions as a stable electrocatalyst for the oxygen reduction reaction†","authors":"Nannan Jiang, Hao Wang, Huihui Jin, Xuwei Liu and Lunhui Guan","doi":"10.1039/D4EY00194J","DOIUrl":"https://doi.org/10.1039/D4EY00194J","url":null,"abstract":"<p >Platinum dissolution is one of the primary factors affecting the stability of Pt-based catalysts for the oxygen reduction reaction (ORR) in proton exchange membrane fuel cells (PEMFCs). It is a significant challenge to prevent the dissolution of Pt and enhance the durability of Pt-based catalysts. In this study, we employed a one-step rapid Joule thermal shock method to fabricate a stable ORR catalyst with embedded Pt<small>₅</small>Ce alloy (E-Pt<small>₅</small>Ce). The strong catalyst-support interactions between the Pt–C layer suppress particle agglomeration and Ostwald ripening, and its steric hindrance effect reduces the electronic density at Pt sites, decreasing the adsorption energy of Pt with oxygen-containing intermediates and preventing Pt dissolution. The Pt–C layer also increases the accessibility of active sites, boosting the ORR activity. In acidic media, E-Pt<small>₅</small>Ce shows a mass activity (MA) and specific activity (SA) of 2.86 A mg<small>_Pt</small><small>⁻¹</small> and 2.03 mA cm<small>⁻²</small>, outperforming the commercial Pt/C by factors of approximately 15 and 5, respectively. When used as a cathode catalyst for a PEMFC, the MA at 0.90 V is almost twice the DOE 2025 target. After stability testing, there is no prominent loss in catalytic activity. Density functional theory calculations confirm that the Pt–C coordination bonds also serve as reactive sites. This work uncovers the mechanism of action of the Pt–C coordination layer, which plays a crucial role in the preparation and performance of ORR catalysts.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 6","pages":" 1253-1262"},"PeriodicalIF":0.0,"publicationDate":"2024-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d4ey00194j?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142565682","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Efficient CO2-to-CO conversion in dye-sensitized photocatalytic systems enabled by electrostatically-driven catalyst binding†","authors":"Vasilis Nikolaou, Palas Baran Pati, Hélène Terrisse, Marc Robert and Fabrice Odobel","doi":"10.1039/D4EY00156G","DOIUrl":"https://doi.org/10.1039/D4EY00156G","url":null,"abstract":"<p >The development of noble metal-free dye-sensitized photocatalytic systems (DSPs) for CO<small>₂</small>-to-CO conversion remains limited. Current literature primarily focuses on a single strategy: the simultaneous loading of both the photosensitizer (PS) and the catalyst (CAT) onto titanium dioxide nanoparticles (TiO<small>₂</small> NPs) using anchoring groups. Here, we introduce an innovative method through immobilizing a positively-charged molecular CAT onto negatively-charged PS–TiO<small>₂</small> NPs. Our approach yields promising results, including near-complete CO<small>₂</small>-to-CO conversion (∼100% CO) and exceptional stability, achieving 1658 turnover numbers <em>versus</em> the CAT and an apparent quantum yield efficiency (AQY) of 16.9%.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 6","pages":" 1314-1319"},"PeriodicalIF":0.0,"publicationDate":"2024-09-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d4ey00156g?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142565689","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Green energy driven methane conversion under mild conditions","authors":"Jiakang You, Yifan Bao, Yanzhao Zhang, Muxina Konarova, Zhiliang Wang and Lianzhou Wang","doi":"10.1039/D4EY00155A","DOIUrl":"10.1039/D4EY00155A","url":null,"abstract":"<p >Methane is a critical energy resource but also a potent greenhouse gas, significantly contributing to global warming. To mitigate the negative effect of methane, it is meaningful to explore an effective methane conversion process motivated with green energy such as green electricity and sunlight. The selectivity and production rate are the key criteria in methane conversion. This review provides a comprehensive overview of recent efforts and understanding in methane conversion to valuable products, including oxygenates and hydrocarbons, by taking advantage of electrocatalysis and photocatalysis. The review begins with a general understanding of C–H bond activation mechanisms. It then focuses on electrocatalytic methane conversion (EMC) with an emphasis on catalyst design for oxygenate production, and photocatalytic methane conversion (PMC) with a particular focus on hydrocarbon production, especially ethylene (C<small>₂</small>H<small>₄</small>), due to the differences in oxygen sources between the two systems. An in-depth understanding of EMC and PMC mechanisms is also discussed to provide insights for improved catalyst design aimed at selective product generation. Finally, successful catalyst designs for EMC and PMC are summarized to identify challenges in achieving highly efficient and selective production of value-added chemicals and to offer clear guidance for future research efforts in green methane conversion.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 6","pages":" 1210-1227"},"PeriodicalIF":0.0,"publicationDate":"2024-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d4ey00155a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142225094","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Catalytic fast pyrolysis of cellulose to oxygenates: roles of homogeneous and heterogeneous catalysts","authors":"Yingchuan Zhang, Zijing Li, Tao Zhou and Guangri Jia","doi":"10.1039/D4EY00154K","DOIUrl":"10.1039/D4EY00154K","url":null,"abstract":"<p >Catalytic fast pyrolysis (CFP) of biomass is an efficient approach that can overcome the structural recalcitrance of solid biomass (<em>e.g.</em>, crystalline cellulose) to produce sugar monomers and their derivatives within seconds. The composition of the product mixture, which is accumulated in a liquid called bio-oil, is highly tuneable through the use of <em>in situ</em>/<em>ex situ</em> catalysts for the downstream production of sustainable fuels and fine chemicals. This minireview summarises the recent advances in homogeneous and heterogeneous catalysts in the CFP production of versatile oxygenates as fuel precursors or bulk chemicals. First, a brief overview of primary CFP pathways, including cellulose-to-levoglucosan (LGA) conversion and the production of three important derivative anhydrosugars, is provided. Particular attention is paid to the roles of homogeneous and heterogeneous catalysts in promoting secondary reforming of LGA by dehydration and to alternative pathways <em>via</em> C3–C6 cyclisation or benzylic rearrangement over versatile catalysts (<em>e.g.</em>, aqueous acids, zeolites, metal oxides) with Brønsted/Lewis acidity to produce a variety of oxygenates in bio-oil. This minireview may provoke more CFP technologies by clarifying the opportunities and challenges in the selective production of different reformed oxygenates, complementing CFP-based production of aromatics from biomass.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 6","pages":" 1238-1246"},"PeriodicalIF":0.0,"publicationDate":"2024-09-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d4ey00154k?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142197054","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}