Krista Kuutti, Manoj Kumar Ghosalya, Paavo Porri, Jacopo De Bellis, Päivi Jokimies, Harishchandra Singh, Shubo Wang, Graham King, Javier Fernández-Catalá, Ferdi Schüth, Kaisu Ainassaari, Mika Huuhtanen, Marko Huttula, Samuli Urpelainen and Sari Rautiainen
{"title":"Mechanochemical synthesis of Pt/TiO2 for enhanced stability in dehydrogenation of methylcyclohexane†","authors":"Krista Kuutti, Manoj Kumar Ghosalya, Paavo Porri, Jacopo De Bellis, Päivi Jokimies, Harishchandra Singh, Shubo Wang, Graham King, Javier Fernández-Catalá, Ferdi Schüth, Kaisu Ainassaari, Mika Huuhtanen, Marko Huttula, Samuli Urpelainen and Sari Rautiainen","doi":"10.1039/D5CY00173K","DOIUrl":"https://doi.org/10.1039/D5CY00173K","url":null,"abstract":"<p >Catalytic hydrogenation/dehydrogenation of liquid organic hydrogen carriers (LOHCs), such as methylcyclohexane (MCH), enables versatile and safe transport and storage of hydrogen as a carbon neutral fuel. Supported platinum catalysts are commonly used for the dehydrogenation reaction, however, they often suffer from loss of activity due to coking. Herein, we present mechanochemically synthesised platinum on titania catalyst for the dehydrogenation of MCH, prepared starting only from metallic platinum and titania. Dry mechanochemical catalyst syntheses do not produce waste waters or toxic fumes, which are generated in the deposition of metal precursors by conventional wet synthesis methods. Detailed characterisation of the catalysts revealed that ball milling produced highly dispersed nanoparticles. Furthermore, continuous-flow MCH dehydrogenation experiments showed that the mechanochemically prepared Pt catalyst exhibited improved selectivity and stability compared to a conventional impregnated Pt/TiO<small><sub>2</sub></small> catalyst. The hydrogen production rate of the novel ball-milled catalyst was among the highest reported for dehydrogenation of methylcyclohexane, 670 mmol<small><sub>H<small><sub>2</sub></small></sub></small> g<small><sub>Pt</sub></small><small><sup>−1</sup></small> min<small><sup>−1</sup></small>.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 14","pages":" 4143-4155"},"PeriodicalIF":4.4,"publicationDate":"2025-06-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/cy/d5cy00173k?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144624107","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}
Sophie H. Dewick, Thomas M. Hood, Yisong Han, Steven Huband and Adrian B. Chaplin
{"title":"Rhodium-catalysed hydrogenation of nitrous oxide†","authors":"Sophie H. Dewick, Thomas M. Hood, Yisong Han, Steven Huband and Adrian B. Chaplin","doi":"10.1039/D5CY00490J","DOIUrl":"https://doi.org/10.1039/D5CY00490J","url":null,"abstract":"<p >We report on the discovery of “hidden” heterogeneous catalysis in the hydrogenation of nitrous oxide while assessing the catalytic activity of a rhodium(<small>I</small>) hydride complex supported by a nominally robust phosphine-based pincer ligand. Commercially available [Rh(COD)(OH)]<small><sub>2</sub></small> was subsequently identified as a more effective catalyst precursor, enabling the hydrogenation of nitrous oxide with an apparent turnover number >3000 at room temeprature.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 14","pages":" 4126-4129"},"PeriodicalIF":4.4,"publicationDate":"2025-06-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/cy/d5cy00490j?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144624105","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}
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
{"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><sub>2</sub></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><sup>2+</sup></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><sup>−1</sup></small> h<small><sup>−1</sup></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><sub>2</sub></small>, corresponding to an enhancement in its catalytic activity. The mechanism of CO<small><sub>2</sub></small> catalytic reduction showed that *COOH and *CHO are the key intermediates in the rate-controlling steps in the CO<small><sub>2</sub></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}
Jung Lin Wong, Jiuan Jing Chew, Basil T. Wong, Femiana Gapsari, Diah Agustina Puspitasari and Jaka Sunarso
{"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}
Kang Rui Garrick Lim, Toghrul Azizli, Selina K. Kaiser, Michael Aizenberg, Matthew M. Montemore and Joanna Aizenberg
{"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><sub>2</sub></small>Au<small><sub>98</sub></small>/SiO<small><sub>2</sub></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}
Samira Motamednejad, Reza Panahi, Kourosh Tabar Heydar, Li Gao, Bingsen Zhang and Mozaffar Shakeri
{"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><sup>2</sup></small> g<small><sup>−1</sup></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><sub>4</sub></small><small><sup>+</sup></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}
Quanjin Wang, Mingming Qin, Qian Wang, Kaiming Wang and Zhiqi Cong
{"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><sub>2</sub></small>O<small><sub>2</sub></small>-dependent P450 steroid dihydroxylase through rational engineering of the H<small><sub>2</sub></small>O<small><sub>2</sub></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><sub>cat</sub></small>/<em>K</em><small><sub>m</sub></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><sub>2</sub></small>O/H<small><sub>2</sub></small>O<small><sub>2</sub></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}
Chuanyi Xiong, Huayu Liang, Yinwu Li and Zhuofeng Ke
{"title":"The critical role of boron hybridization (sp3vs. sp2vs. sp) in hydrogenation mechanisms by boron-based Ru catalysts†","authors":"Chuanyi Xiong, Huayu Liang, Yinwu Li and Zhuofeng Ke","doi":"10.1039/D5CY00380F","DOIUrl":"https://doi.org/10.1039/D5CY00380F","url":null,"abstract":"<p >Boron–transition metal (B–TM) catalysts have emerged as promising systems for hydrogenation reactions due to their unique bifunctional reactivity. However, the electronic structure–activity relationships of B–TM systems with different boron hybridizations remain poorly understood. This study systematically investigates how the sp<small><sup>3</sup></small>, sp<small><sup>2</sup></small>, and sp hybridizations influence the catalytic mechanisms of B–Ru complexes in hydrogen activation and ethylene hydrogenation. For hydrogen activation, the sp<small><sup>3</sup></small>-B–Ru system follows a hydride mechanism (Δ<em>G</em> = 31.2 kcal mol<small><sup>−1</sup></small>), while sp<small><sup>2</sup></small>/sp-B–Ru systems adopt a more efficient proton mechanism with lower barriers (15.3 and 20.8 kcal mol<small><sup>−1</sup></small>, respectively). Orbital analysis demonstrates that the Ru contribution to bridging hydrides increases progressively from sp<small><sup>3</sup></small> (9.4%) to sp (13.9%) systems, correlating with enhanced catalytic activity. For the hydrogenation reaction, the 2c–2e terminal is more favorable than the 3c–2e bridging hydrogen mechanism. Moreover, in the bridging hydrogen mechanism, the metal oxidation state remains unchanged for the sp<small><sup>2</sup></small> and the sp systems, which is superior to that for the sp<small><sup>3</sup></small> system. These findings provide molecular-level insights for the rational design of B–TM catalysts with improved hydrogenation performance.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 13","pages":" 3906-3917"},"PeriodicalIF":4.4,"publicationDate":"2025-06-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144514483","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}
Jiajun Du, Jun Deng, ChangAn Zhou, Hairong Yue, Chong Liu, Patrik Schmuki, Štěpán Kment and Xuemei Zhou
{"title":"Regulating protonation paths for enhanced photocatalytic CO2 methanation by coupling Pt sites on WO2.9/TiO2†","authors":"Jiajun Du, Jun Deng, ChangAn Zhou, Hairong Yue, Chong Liu, Patrik Schmuki, Štěpán Kment and Xuemei Zhou","doi":"10.1039/D5CY00167F","DOIUrl":"https://doi.org/10.1039/D5CY00167F","url":null,"abstract":"<p >CO<small><sub>2</sub></small> methanation <em>via</em> photocatalysis with water vapor is a sustainable technique for reducing CO<small><sub>2</sub></small> emission but is challenged by the high energy barrier associated with the initial adsorption, activation and protonation of CO<small><sub>2</sub></small> molecules. In this work, a substoichiometric WO<small><sub>2.9</sub></small> thin film with strong Lewis acidity was coated on TiO<small><sub>2</sub></small> microspheres, followed by the deposition of Pt cocatalysts on WO<small><sub>2.9</sub></small> with controlled Pt single atoms and clusters (Pt–WO<small><sub>2.9</sub></small>/TiO<small><sub>2</sub></small>). The methane production rate reached 10.74 μmol h<small><sup>−1</sup></small> g<small><sup>−1</sup></small> with a selectivity of 99.8%, which was ∼40 times higher than that of bare TiO<small><sub>2</sub></small> (0.27 μmol h<small><sup>−1</sup></small> g<small><sup>−1</sup></small>). The high methane production rate was attributed to the synergy of Pt sites on the WO<small><sub>2.9</sub></small>/TiO<small><sub>2</sub></small> heterojunction, where the Pt clusters facilitated water dissociation, thereby providing H* through hydrogen spillover on the surface, and the presence of a substoichiometric WO<small><sub>2.9</sub></small> surface further enhanced the spillover process. The high density of active H* promoted the protonation pathway for CO<small><sub>2</sub></small> activation (CO<small><sub>2</sub></small> → COOH<small><sup>+</sup></small> → *COOH), which improved the adsorption of the essential intermediate *CO on Pt single atoms and displayed a significantly reduced energy barrier for the protonation reaction of C1 intermediates, resulting in a mixed reaction pathway. This work provides new insights into a mechanism to regulate the reaction path to facilitate efficient photocatalytic CO<small><sub>2</sub></small> methanation.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 13","pages":" 4002-4011"},"PeriodicalIF":4.4,"publicationDate":"2025-06-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144514485","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}
Weiguang Fang, Jun Zhu, Shan Gao, Juanjuan Zhao, Na Li, Shoujie Liu and Mingzai Wu
{"title":"Hierarchical construction of Co nanoparticles embedded in an N doped carbon nanotube/porous nanosheet electrocatalyst for Zn–air batteries†","authors":"Weiguang Fang, Jun Zhu, Shan Gao, Juanjuan Zhao, Na Li, Shoujie Liu and Mingzai Wu","doi":"10.1039/D5CY00483G","DOIUrl":"https://doi.org/10.1039/D5CY00483G","url":null,"abstract":"<p >Inefficient cathodic reactions severely limit the practical performance of rechargeable zinc–air batteries (RZABs) and become a fundamental bottleneck in their development. The exploitation of cost-effective cathode electrocatalysts is significant for addressing this issue. Herein, we demonstrate a facile programmed annealing strategy to fabricate an efficient electrocatalyst with a structure of Co nanoparticles embedded in N doped carbon nanotubes/porous nanosheets (Co@DUGC). Benefiting from the <em>in situ</em> wrapped Co nanoparticles and doped N as catalytic and adsorptive sites, and a hierarchical carbon nanotube/porous nanosheet architecture for fast electron transfer and mass diffusion, the fabricated Co@DUGC exhibits excellent bifunctional electrocatalytic performance with a positive half-wave potential of 0.87 V in the ORR and a low overpotential of 414 mV in the OER. As a cathodic catalyst, Co@DUGC endows a home-made liquid RZAB with a high peak power density of 150 mW cm<small><sup>−2</sup></small>, a large specific discharge capacity of 816.9 mA h g<small><sub>Zn</sub></small><small><sup>−1</sup></small> and a durable rechargeability of 314 cycles. Meanwhile, a button RZAB based on Co@DUGC displays a peak power density of 85.3 mW cm<small><sup>−2</sup></small>, a specific discharge capacity of 643.7 mA h g<small><sub>Zn</sub></small><small><sup>−1</sup></small> and a charge–discharge cycle life over 95 times, revealing its reliability for portable applications. This work demonstrates a convenient and rational design of transition metal decorated carbon electrocatalysts for high-performance RZABs.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 14","pages":" 4291-4302"},"PeriodicalIF":4.4,"publicationDate":"2025-06-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144624121","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}