Catalysis Science & Technology最新文献

{"title":"Cobalt-ion center engineering in ZIF-67 for enhanced photothermal catalytic CO2 reduction: mechanistic insights into intermediate regulation and activity optimization","authors":"Bin Guan, Junyan Chen, Lei Zhu, Zhongqi Zhuang, Xuehan Hu, Chenyu Zhu, Sikai Zhao, Kaiyou Shu, Hongtao Dang, Junjie Gao, Luyang Zhang, Tiankui Zhu, Wenbo Zeng, Minfan Qian, Zhangtong Li, Yang Lu, Shuai Chen and Zhen Huang","doi":"10.1039/D5CY00395D","DOIUrl":"https://doi.org/10.1039/D5CY00395D","url":null,"abstract":"<p >Herein, a detailed study of ZIF-67 CO<small>₂</small> photothermal reduction catalysts was carried out, including the characterization of their physicochemical properties, photothermal catalytic performances and reaction mechanisms. Through the systematic characterization of ZIF-67 catalyst samples, the differences in their crystal structures, morphological features, specific surface areas and optical properties were investigated. In addition, the catalytic mechanism of the catalysts was investigated in detail by <em>in situ</em> DRIFTS and DFT calculations. The experimental results showed that among the ZIF-67 catalyst prepared with different ratios of Co<small>²⁺</small> and 2-MI precursors, the ZIF-67 (8–1) catalyst exhibited an distinct crystal lattice structure, strongest photoelectron transfer ability, and largest specific surface area, resulting in an optimal catalytic activity (total yield = 4.71 μmol g<small>⁻¹</small> h<small>⁻¹</small>). The band gap width of this material could be controlled by regulating the content of Co metal-ion centers to promote the photogenerated charge transfer in the adsorption–reduction process of CO<small>₂</small>, corresponding to an enhancement in its catalytic activity. The mechanism of CO<small>₂</small> catalytic reduction showed that *COOH and *CHO are the key intermediates in the rate-controlling steps in the CO<small>₂</small> catalytic reduction reaction, and the energy barrier of the former controlled the reaction product yield, while that of the latter was the key to regulate product selectivity.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 14","pages":" 4303-4318"},"PeriodicalIF":4.4,"publicationDate":"2025-06-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144624122","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":"Modified indophenol blue method enables reliable routine quantification of photocatalytically produced ammonia in aqueous sulfite electrolyte†","authors":"Jingfu Sun, Xiaoyu Zhang, Jingwen Mu, Xi Han and Yaoguang Yu","doi":"10.1039/D5CY00491H","DOIUrl":"https://doi.org/10.1039/D5CY00491H","url":null,"abstract":"<p >Extensive research efforts in the chemical engineering community have been devoted to transforming the ammonia synthesis process from the energy-intensive and capital-heavy Haber–Bosch method to alternative green production methods. Photocatalytic and photoelectrochemical methods have emerged as pivotal alternative strategies attributed to environmental sustainability. Sulfides are vital photoactive materials with potential in photocatalytic and photoelectrochemical water splitting and CO<small>₂</small> reduction, aided by economic sacrificial reagents like sulfite to prevent photocorrosion. However, most of the previously reported ammonia quantification methods in aqueous sulfite electrolyte systems malfunction due to high concentrations of Na<small>⁺</small> or K<small>⁺</small> ions or reactions between sulfite ions, sulfide ions, and chromogenic reagents. These obstacles exclude sulfide catalysts from photocatalytic and photoelectrochemical ammonia synthesis, significantly hindering field development. We developed a modified indophenol blue method to reliably and economically quantify ammonia in aqueous sulfite electrolyte using the advanced oxidation method. Furthermore, a standardized operating procedure is established to eliminate potential false-positive results. This work not only provides guidance to reliably and economically quantify ammonia in aqueous sulfite electrolyte but also paves the way for the development of advanced sulfide catalysts for photocatalytic and photoelectrochemical ammonia synthesis applications.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 15","pages":" 4542-4549"},"PeriodicalIF":4.4,"publicationDate":"2025-06-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144714618","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":"Dual-mode catalytic degradation of diclofenac by copper oxide-modified TiO2/MnOx composites: insights from dark and UV-A activation†","authors":"Gloria Issa, Sylvie Kříženecká, Petr Bezdička, Daniela Popelková, Martin Kormunda, Jakub Ederer, Daniel Bůžek, Jan Čundrle, Zdeněk Baďura, Jiří Henych and Martin Šťastný","doi":"10.1039/D4CY01400F","DOIUrl":"https://doi.org/10.1039/D4CY01400F","url":null,"abstract":"<p >Diclofenac sodium (DCF), a widely used nonsteroidal anti-inflammatory drug, is a persistent pharmaceutical contaminant that resists removal by conventional wastewater treatment. In this study, CuO-modified TiO<small>₂</small>/MnO<small>_<em>x</em></small> composites were developed as multifunctional catalysts for DCF degradation under both dark and UV-A conditions. The materials exhibited dual-mode reactivity through distinct mechanisms: (i) non-radical oxidative degradation under dark conditions, and (ii) radical-mediated photocatalysis under UV-A irradiation. Under illumination, the formation of an interfacial p–n–p heterojunction between CuO, MnO<small>_<em>x</em></small>, and TiO<small>₂</small> generated internal electric fields that directed charge carrier migration—electrons flowing from the conduction band of TiO<small>₂</small> toward CuO and MnO<small>_<em>x</em></small> domains, and holes in the reverse direction. This spatial charge separation suppressed recombination and sustained redox cycling between Cu<small>²⁺</small>/Cu<small>⁺</small> and Mn<small>⁴⁺</small>/Mn<small>³⁺</small>, promoting continuous ROS generation. In the absence of light, DCF degradation proceeded <em>via</em> non-radical oxidative pathways involving surface-bound reactive oxygen species and redox-active metal centers. Surface-sensitive XPS and hydroxyl quantification (TOTH) revealed elevated Mn<small>³⁺</small>/Mn<small>⁴⁺</small> ratios, enriched surface-associated lattice oxygen, and high –OH group densities for the most active catalysts. These features collectively facilitated pollutant adsorption, oxygen activation, and sustained interfacial electron transfer. LC-MS/MS analysis confirmed a consistent degradation pathway across both regimes, involving hydroxylation, decarboxylation, and dechlorination of DCF. The Cu/5Ti5Mn-HT and Cu/8Ti2Mn-HT catalysts achieved exceptional dark-phase degradation efficiencies (∼99.8% and ∼99.4%, respectively), while Cu/TiO<small>₂</small> exhibited the highest UV-A photocatalytic performance (∼42%). These findings demonstrate the synergistic advantage of redox-active metal oxides and interfacial design, establishing CuO–MnO<small>_<em>x</em></small>–TiO<small>₂</small> composites as promising candidates for advanced pharmaceutical pollutant remediation.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 15","pages":" 4438-4456"},"PeriodicalIF":4.4,"publicationDate":"2025-06-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/cy/d4cy01400f?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144714602","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":"Strongly acidic SSZ-13 zeolite boosts high-space-velocity CO2-to-light olefin conversion via synergistic bifunctional catalysis†","authors":"Xiangzeng Chen, Jiejie Ling, Yan Gao, Ming-Ao Sun, Jilong Wang and Le Xu","doi":"10.1039/D5CY00512D","DOIUrl":"https://doi.org/10.1039/D5CY00512D","url":null,"abstract":"<p >The direct conversion of CO<small>₂</small> to light olefins has gained significant attention in C1 chemistry. Compared to the modified Fischer–Tropsch synthesis route (CO<small>₂</small>-FTO), the oxide–zeolite (OXZEO) composite catalytic system—which integrates methanol synthesis with methanol-to-olefin (MTO) reaction—has demonstrated superior light olefin selectivity. Nevertheless, conventional OXZEO systems employing silicoaluminophosphate (SAPO) zeolites face serious limitations due to their inherent weak acidity, requiring relatively low space velocities for effective MTO catalysis and resulting in suboptimal light olefin space-time-yield (STY). We developed a bifunctional ZnZrO<small>_<em>x</em></small>/H-SSZ-13 system where CO<small>₂</small> hydrogenates to methanol on ZnZrO<small>_<em>x</em></small>, then rapidly converts to olefins on the strongly acidic zeolite. Crucially, the strong acidity of the SSZ-13 zeolite enables effective methanol conversion even at elevated space velocities. This system achieved 7.50 mmol g<small>_cat</small><small>⁻¹</small> h<small>⁻¹</small> light olefin STY under a low reaction pressure of 1 MPa and a high gas-hourly-space-velocity (GHSV) of 21 000 mL g<small>_cat</small><small>⁻¹</small> h<small>⁻¹</small>, with 82.6% light olefin selectivity. This work highlights the critical synergy between tailored acid strength of the zeolite component and reaction conditions in advancing CO<small>₂</small>-to-olefin catalysis.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 15","pages":" 4575-4587"},"PeriodicalIF":4.4,"publicationDate":"2025-06-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144714620","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":"On-site catalytic dehydrogenation of methylcyclohexane: mechanisms, catalysts, advances, and prospects†","authors":"Jung Lin Wong, Jiuan Jing Chew, Basil T. Wong, Femiana Gapsari, Diah Agustina Puspitasari and Jaka Sunarso","doi":"10.1039/D5CY00333D","DOIUrl":"https://doi.org/10.1039/D5CY00333D","url":null,"abstract":"<p >The storage and transport of hydrogen in the form of chemicals, such as ammonia, methanol, and liquid organic hydrogen carrier (LOHC), has emerged as a promising technology as they can be stored under milder conditions than compressed hydrogen and liquefied hydrogen. Methylcyclohexane (MCH)–toluene (TOL) emerged as a prominent LOHC system with moderate melting point, hydrogen capacity, and mild storage conditions. This review provides an overview of existing hydrogen storage technologies, followed by a focused discussion different LOHC systems, with an emphasis on MCH as a promising LOHC, its dehydrogenation reaction mechanism and the performance of the available catalysts. The purpose of this review is to critically assess the latest developments regarding the catalytic dehydrogenation of MCH. The effects of various catalysts and operating conditions on the dehydrogenation performance of MCH, coupled with technical, economic, and environmental perspectives of the MCH-based hydrogen supply chain, were presented. This work also highlights the obstacles associated with using MCH as a hydrogen carrier for on-site dehydrogenation at fuel stations. Additionally, this review discusses the current stage of commercialisation of MCH as a hydrogen carrier in the Asia-Pacific region.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 14","pages":" 4063-4084"},"PeriodicalIF":4.4,"publicationDate":"2025-06-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144624102","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":"Near-infrared-activated NaYF4:Yb3+,Tm3+@g-C3N4@WO3@MXene photocatalytic system for enhanced removal of tetracycline antibiotics†","authors":"Yuangong Ma, Youlin Huang, Wensheng Zhang, Dongfang Han and Li Niu","doi":"10.1039/D5CY00480B","DOIUrl":"https://doi.org/10.1039/D5CY00480B","url":null,"abstract":"<p >To utilize near-infrared (NIR) light within the solar energy spectrum, we have engineered an advanced composite of NaYF<small>₄</small>:Yb<small>³⁺</small>,Tm<small>³⁺</small>@g-C<small>₃</small>N<small>₄</small>@WO<small>₃</small>@MXene (denoted as NYT@g-C<small>₃</small>N<small>₄</small>@WO<small>₃</small>@MXene) capable of absorbing NIR light to facilitate photocatalytic reactions. This environmentally benign system integrates semiconductor heterostructures (g-C<small>₃</small>N<small>₄</small> and WO<small>₃</small>) with upconversion nanoparticles (NaYF<small>₄</small>:Yb<small>³⁺</small>,Tm<small>³⁺</small>, abbreviated as NYT) and Ti<small>₃</small>C<small>₂</small> MXene nanosheets. Experimental validation demonstrated exceptional performance in antibiotic remediation, with the composite achieving 86.3% tetracycline decomposition over 12 hours under NIR irradiation through synergistic mechanisms, while also exhibiting good cycling stability. The enhanced photocatalytic activity arises from collaborative effects between upconversion luminescence, optimized charge transfer pathways within the heterojunction architecture, and the visible light absorption characteristics of MXene.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 15","pages":" 4588-4598"},"PeriodicalIF":4.4,"publicationDate":"2025-06-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144714621","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":"Effects of Pd ensemble size in dilute and single atom alloy PdAu catalysts for one-pot selective hydrogenation and reductive amination†","authors":"Kang Rui Garrick Lim, Toghrul Azizli, Selina K. Kaiser, Michael Aizenberg, Matthew M. Montemore and Joanna Aizenberg","doi":"10.1039/D5CY00441A","DOIUrl":"https://doi.org/10.1039/D5CY00441A","url":null,"abstract":"<p >In the one-pot reaction between nitroarenes, aldehydes, and hydrogen, the desired outcome is the selective hydrogenation of nitroarenes to form aminoarenes that condense with aldehydes to yield pharmaceutically relevant imines and <em>N</em>-alkylamines. One approach to facilitate the selective hydrogenation of nitroarenes over aldehydes involves using bimetallic catalysts with near equimolar ratios. However, structural characterization of metallic ensembles on the nanoparticle surface is challenging at such high alloying ratios, which hinders the elucidation of clear structure–property relationships. Here, we prepared a well-controlled series of dilute Pd-in-Au alloy catalysts with a fixed nanoparticle size as a model system to investigate the effects of surface Pd ensemble size, from single atoms to dimers and trimers, in the one-pot hydrogenation reaction between nitrobenzene and benzaldehyde as our probe reaction. The highest (near unity) selectivity to condensation products was achieved using the catalyst with the lowest Pd content prepared (Pd<small>₂</small>Au<small>₉₈</small>/SiO<small>₂</small>), which predominantly exposed Pd single atoms on the nanoparticle surface as verified by surface-sensitive spectroscopy. Theoretical calculations reveal that Pd single atoms were inactive for benzaldehyde adsorption and thus enabled selective nitrobenzene hydrogenation. On the contrary, the adsorption of benzaldehyde became stronger than nitrobenzene for Pd trimers and larger ensembles, explaining the enhanced competitive adsorption from benzaldehyde in catalysts with increasing Pd content. Our results demonstrate that the commonly used (near equimolar) alloying ratio is rather arbitrary and may not necessarily produce the highest selectivity to condensation products. Instead, we illustrate how controlling the nanoscale Pd ensemble size on the nanoparticle surface tunes competitive kinetics to steer selectivity towards forming the desired condensation products.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 14","pages":" 4179-4193"},"PeriodicalIF":4.4,"publicationDate":"2025-06-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144624134","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":"Maximizing light olefin production in the cracking of polyethylene using hierarchical acidic–basic zeolites†","authors":"Samira Motamednejad, Reza Panahi, Kourosh Tabar Heydar, Li Gao, Bingsen Zhang and Mozaffar Shakeri","doi":"10.1039/D5CY00310E","DOIUrl":"https://doi.org/10.1039/D5CY00310E","url":null,"abstract":"<p >Fast coking, low selectivity to light olefins, and expensive synthesis are the challenges of FAU-type zeolites in the cracking of plastic waste. We addressed these problems by a one-pot seed-assisted synthesis of hierarchical acidic–basic zeolites using silica completely extracted from a highly impure kaolin containing alkali and alkaline earth metals and quartz minerals and investigating their structural stability and catalytic performance in the cracking of polyethylene. The resulting NaY zeolites, which had excellent surface areas of 509–635 m<small>²</small> g<small>⁻¹</small>, inherited morphology, crystallinity, silicon-to-aluminum ratio (3.3 to 10.52), hierarchical structure, and reduced particle size from the seeds and the basicity from the homogeneously distributed alkali and alkaline earth metals, inducing distinctive structural and catalytic properties. For example, calcining the NH<small>₄</small><small>⁺</small>-exchanged zeolites into their HY form significantly reduced their crystallinity and etched microporosity while preserving morphology, resulting in a high Al content and well-defined mesoporous aluminosilicate materials. We then looked at the causes of susceptibility to protonation and how to stabilize their structure. Compared with the reference acidic HY zeolite, hierarchical zeolites and mesoporous aluminosilicates possessing enhanced basicity yielded a comparable activity, eight times less coke, and up to twice the olefin production in the cracking of polyethylene. When compared to the acidic HY zeolite, the acidic–basic catalysts generated liquid oils of significantly higher quality, with a composition lacking in naphthalene (3.08 <em>vs.</em> 62.44%) and enriched in long-chain olefins (80.5% <em>vs.</em> 1%). The hydrogen transfer coefficients for the hierarchical acidic–basic zeolites were much smaller than that of the reference acidic HY zeolite (0.037–0.17 <em>vs.</em> 1.59), suggesting dominance of the monomolecular over the bimolecular cracking mechanism by the former catalysts. The acidic–basic hierarchical HY zeolites and mesoporous aluminosilicates displayed a stable mesostructure with improved selectivity and activity over regeneration and reuse. These results showed the possibility of turning the drawback of impurities in kaolin into improved basicity and mesoporosity advantages to maximize olefin production and minimize coke formation in the cracking of plastic waste by zeolites.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 14","pages":" 4156-4169"},"PeriodicalIF":4.4,"publicationDate":"2025-06-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144624132","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":"Rationally engineering an H2O2-dependent P450 dihydroxylase for steroid functionalisation†","authors":"Quanjin Wang, Mingming Qin, Qian Wang, Kaiming Wang and Zhiqi Cong","doi":"10.1039/D5CY00504C","DOIUrl":"https://doi.org/10.1039/D5CY00504C","url":null,"abstract":"<p >P450-catalysed steroid hydroxylation serves as both a fundamental biochemical pathway for <em>in vivo</em> steroid hormone biosynthesis and metabolism, and a pivotal tool for the biotechnological production of steroidal pharmaceuticals. Herein, we report the construction of an efficient H<small>₂</small>O<small>₂</small>-dependent P450 steroid dihydroxylase through rational engineering of the H<small>₂</small>O<small>₂</small> tunnel, guided by molecular dynamics (MD) simulations and crystallographic analysis. The triple mutant F184A/F191A/E196A demonstrated an approximately 80-fold enhancement in catalytic efficiency (<em>k</em><small>_cat</small>/<em>K</em><small>_m</small>) for testosterone hydroxylation compared to wild-type CYP105D18, indicating a dramatic improvement in peroxygenase activity. Testosterone hydroxylation by this mutant predominantly yielded 2β-hydroxytestosterone (81%), with minor 16α-hydroxytestosterone (19%). Notably, the 2β-hydroxylated product could be quantitatively converted to 2β,15α-dihydroxytestosterone in the subsequent reaction. This study provides novel insights into the stepwise design of H<small>₂</small>O/H<small>₂</small>O<small>₂</small> tunnels in P450 enzymes through the integration of MD simulations and crystallographic data. Furthermore, it establishes a practical enzymatic approach for the regio- and stereoselective dihydroxylation of steroids, with potential applications in pharmaceutical synthesis.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 14","pages":" 4170-4178"},"PeriodicalIF":4.4,"publicationDate":"2025-06-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144624133","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":"C–C coupling regulation to enhance the stability of ambient pressure photothermal CO2 hydrogenation to multi-hydrocarbon compounds†","authors":"Xianhua Bai, Linjia Han, Jialin Wang, Yanhong Luo, Yiming Li, Jiangjian Shi, Yaguang Li, Dongmei Li and Qingbo Meng","doi":"10.1039/D5CY00535C","DOIUrl":"https://doi.org/10.1039/D5CY00535C","url":null,"abstract":"<p >Ambient pressure photothermal CO<small>₂</small> hydrogenation for producing multi-hydrocarbon (C<small>₂₊</small>: C<small>_<em>x</em></small>H<small>_<em>y</em></small>, where carbon number &gt;1) compounds is a highly valuable way to recycle CO<small>₂</small> and an important path to achieve carbon neutrality. It suffers from carbon deposition during the C–C coupling process that results in low catalytic stability. To overcome this challenge, a Fe<small>₃</small>C/ZnO heterostructure was designed to realize ambient pressure photothermal CO<small>₂</small> hydrogenation that can not only achieve a C<small>₂₊</small> generation rate of ∼1.9 mmol g<small>⁻¹</small> h<small>⁻¹</small>, 67.9% C<small>₂₊</small> selectivity and a CO<small>₂</small> conversion rate of 29.8% under natural sunlight irradiation, but also extend the stable reaction duration from 40 hours to 200 hours. <em>In situ</em> DRIFTS and theoretical calculations demonstrate that the Fe<small>₃</small>C/ZnO heterostructures could significantly reduce the adsorption of CH<small>_<em>x</em></small> intermediates and activate the HCO* intermediates to regulate the C–C formation pathway of photothermal CO<small>₂</small> hydrogenation from the traditional CH<small>_<em>x</em></small> intermediates to HCO* and CO* intermediates, thus mitigating surface carbon deposition. This study contributes to the advancement of new catalysts designed for outdoor photothermal CO<small>₂</small> hydrogenation aimed at robustly producing C<small>₂₊</small> compounds under ambient pressure.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 15","pages":" 4457-4461"},"PeriodicalIF":4.4,"publicationDate":"2025-06-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144714603","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}