EES catalysis最新文献

{"title":"A comparative overview of the electrochemical valorization and incorporation of CO2 in industrially relevant compounds","authors":"Jef R. Vanhoof, Sander Spittaels and Dirk E. De Vos","doi":"10.1039/D4EY00005F","DOIUrl":"10.1039/D4EY00005F","url":null,"abstract":"<p >Climate change is a critical global challenge that requires urgent action to reduce greenhouse gas emissions, including carbon dioxide (CO<small>₂</small>). While essential efforts are being made to reduce emissions by developing new manufacturing processes, it is also crucial to scrutinize sustainable uses for the CO<small>₂</small> that is already produced in excess. The electrochemical CO<small>₂</small> reduction reaction (eCO<small>₂</small>RR) is a highly promising and versatile approach for converting CO<small>₂</small> into valuable base chemicals and fuels, effectively decarbonizing the chemical industry. New methodologies and electrocatalysts in this area are increasingly being investigated, emphasizing the necessary transition to a more sustainable future. In this review, we focus on the eCO<small>₂</small>RR coupled with incorporation in organic or inorganic reactants towards key industrial compounds such as carboxylic acids, ureas and dimethyl carbonate. We provide a broader context by outlining the current industrial synthesis methods of the envisioned compounds. Recent work is summarized in tables for quick comparison while innovations and improvements regarding sustainability and applicability are addressed in more detail.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-02-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d4ey00005f?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139770637","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":"Making light work: designing plasmonic structures for the selective photothermal methanation of carbon dioxide†","authors":"Yi Fen Zhu, Bingqiao Xie, Jodie A. Yuwono, Priyank Kumar, Abhinav S. Sharma, Michael P. Nielsen, Avi Bendavid, Rose Amal, Jason Scott and Emma C. Lovell","doi":"10.1039/D3EY00315A","DOIUrl":"10.1039/D3EY00315A","url":null,"abstract":"<p >Effectively engaging light to induce catalytic activity requires the careful selection of a catalyst support with appropriate and beneficial properties. On this basis, black, plasmonic TiN was employed as a Ni catalyst support for the CO<small>₂</small> methanation reaction under illuminated-only conditions. The positive effects of light illumination were found to be defined by the Ni deposit size and the Ni–TiN interaction. At a high Ni loading (40 wt%, 70 wt%), simulated sunlight induces plasmonic heating through the TiN support which is sufficient to initially <em>in situ</em> reduce the Ni deposits and initiate CO<small>₂</small> methanation. Photothermal effects from TiN and the metallic Ni, combined with reaction exothermicity, then continue to further reduce the Ni and amplify the methanation reaction. At a lower Ni loading (10 wt%), the Ni deposits are smaller and more dispersed. In this case, the topmost Ni deposit surfaces are more strongly influenced by the TiN support due to their closer proximity to the metal–support interface. DFT calculations revealed that this condition can facilitate the migration of light induced plasmonic hot charge carriers from the TiN towards the exposed Ni surface, altering the surface charge of the Ni. The adsorption strength of *CO is subsequently enhanced to enable further reaction rather than desorption as product, thereby boosting CH<small>₄</small> selectivity. The findings discern between the different phenomena (plasmonic heating and hot electron migration) invoked by plasmonic excitation and offer new insight on the contribution these phenomena make to governing catalyst activity and selectivity.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-02-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d3ey00315a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139770636","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":"Multichannel nitrogen-doped carbon fiber confined Fe3C nanoparticles for efficient electroreduction of nitrate†","authors":"Fangzhou Zhang, Zhangsheng Shi, Junliang Chen, Hongxia Luo, Jun Chen and Jianping Yang","doi":"10.1039/D4EY00016A","DOIUrl":"10.1039/D4EY00016A","url":null,"abstract":"<p >Electrochemical conversion of nitrate into benign dinitrogen is a promising solution for water purification and environmental remediation. The development of environmentally friendly electrocatalysts possessing excellent catalytic activity and stability has attracted increasing attention. Herein, a 1D hierarchical architecture with uniformly dispersed Fe<small>₃</small>C nanoparticles confined in multichannel nitrogen-doped carbon fibers (Fe<small>₃</small>C/MNCFs) is reported as a highly efficient NO<small>₃</small>RR electrocatalyst. Fe<small>₃</small>C/MNCFs-800 demonstrates a nitrate conversion of 90.9%, an N<small>₂</small> selectivity of 99.53%, and up to 15 cycles of electrocatalytic stability. The excellent electrocatalytic activity is proposed to be mainly due to the multichannel fibrous architecture beneficial for exposing more active sites and facilitating mass diffusion. Moreover, the strong interaction between active species and fibrous support guarantees the chemical stability and long cycle life. This work provides a reference for the development of high-performance noble-metal-free electrocatalysts for eco-friendly nitrate reduction.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d4ey00016a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139689820","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":"Cu-based catalysts for electrocatalytic nitrate reduction to ammonia: fundamentals and recent advances","authors":"Kouer Zhang, Yun Liu, Zhefei Pan, Qing Xia, Xiaoyu Huo, Oladapo Christopher Esan, Xiao Zhang and Liang An","doi":"10.1039/D4EY00002A","DOIUrl":"10.1039/D4EY00002A","url":null,"abstract":"<p >Electrocatalytic nitrate reduction has been identified as a promising technology for green ammonia production, allowing the conversion of harmful nitrate from wastewater into valuable ammonia using renewable electricity under ambient conditions. Developing advanced electrocatalysts is of paramount significance for improving the ammonia production efficiency in this process. Recently, Cu-based catalysts have been widely investigated in ammonia production <em>via</em> nitrate reduction due to their rapid reduction reaction kinetics, strong electrical conductivity, and ability to inhibit the hydrogen evolution reaction. Meanwhile, the reaction mechanism and computational and experimental methods have been extensively discussed to understand the theory behind the favourable properties of Cu-based catalysts. In this review, we focus on Cu-based catalysts, aiming to provide insights into the latest developments, reaction mechanisms, and state-of-the-art analysis methods for intermediates and products of nitrate reduction to ammonia. Future outlooks and remaining challenges are presented to provide guidance for advancing from experimental explorations to practical applications.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d4ey00002a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139689692","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":"Revisiting group 4–7 transition metals for heterogeneous ammonia synthesis","authors":"Wenbo Gao, Yawei Wang, Qianru Wang, Zhaolong Sun, Jianping Guo and Ping Chen","doi":"10.1039/D3EY00301A","DOIUrl":"10.1039/D3EY00301A","url":null,"abstract":"<p >Ammonia is a key small molecule for manufacturing nitrogen-based fertilizers and organic chemicals and equally important for renewable energy storage and conversion. The available Haber–Bosch ammonia synthesis process using fused iron catalysts operated under harsh conditions is, however, unsustainable. The development of alternative and more efficient approaches to sustainable ammonia production has garnered much attention recently. Most of the prior work has been devoted to the investigation of Fe, Ru or Co-based metal catalysts for ammonia synthesis. In comparison, there are very limited studies on group 4–7 transition metals, because they are prone to form metal nitrides, which are difficult to hydrogenate to ammonia. This mini-review summarizes recent advances in activating these metals for heterogeneous ammonia synthesis. We show that the potential properties of group 4–7 transition metals for ammonia synthesis should be revisited, which may lead to the development of more efficient materials or chemical processes for ammonia production under mild conditions.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d3ey00301a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139658600","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":"Microporous transport layers facilitating low iridium loadings in polymer electrolyte water electrolysis†","authors":"Carl Cesar Weber, Salvatore De Angelis, Robin Meinert, Christian Appel, Mirko Holler, Manuel Guizar-Sicairos, Lorenz Gubler and Felix N. Büchi","doi":"10.1039/D3EY00279A","DOIUrl":"10.1039/D3EY00279A","url":null,"abstract":"<p >Minimizing the power-specific iridium loading in polymer electrolyte water electrolysis (PEWE) is essential for the commercialization and upscaling of this technology. However, decreasing the iridium loading can severely affect performance and stability. Microporous layers (MPL) can overcome some of these issues by maximizing catalyst utilization and increasing cell efficiency. In this study, we combined advanced synchrotron and lab-based X-ray imaging techniques and electrochemical characterization to improve the PEWE cell performance at low Ir loadings using novel MPLs. For the first time, the 3D nanostructure of the catalyst layer was characterized under dry and wet conditions using ptychographic X-ray laminography. We prepared catalyst layers (CL) at three iridium loadings between 2.5 and 0.1 mg<small>_Ir</small>cm<small>⁻²</small> in two different configurations: depositing either on the membrane or on the Ti-substrate (MPL). The MPL structure and catalyst distribution at its surface were analyzed using X-ray tomographic microscopy. Moreover, we investigated the effect of introducing a thin protective Pt coating on the MPL. The electrochemical performance was characterized for all cell combinations, and an in-depth kinetic analysis revealed information on CL utilization. The MPLs exhibit significant benefits for reducing iridium loadings, allowing performance to be sustained with only modest voltage losses. The challenges in fabricating anodic CLs with reduced catalyst loadings and the advantages of using an MPL in both configurations are discussed. The findings of this study contribute to accomplishing the required targets in terms of power-specific iridium loadings for future PEWE systems.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d3ey00279a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139670282","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":"One-dimensional nanotube of a metal–organic framework boosts charge separation and photocatalytic hydrogen evolution from water: synthesis and underlying understanding†","authors":"Lifang Liu, Yejun Xiao, Xiangyang Guo, Wenjun Fan, Nengcong Yang, Chunmei Jia, Shengye Jin and Fuxiang Zhang","doi":"10.1039/D4EY00007B","DOIUrl":"10.1039/D4EY00007B","url":null,"abstract":"<p >One-dimensional (1D) nanostructured inorganic semiconductors have been extensively investigated for efficiently promoting their photocatalytic performances, but it still remains unclear for metal–organic framework (MOF)-based photocatalysis. Herein we present the synthesis 1D Mn-TBAPy MOF nanotubes (denoted as Mn-TBAPy-NT) and give the first demonstration of the marked ability of the 1D nanotube structure to promote charge separation of MOFs relative to that in the Mn-TBAPy single crystal (denoted as Mn-TBAPy-SC), a feature proposed to result from the effect of strain on the nanotubes. As specifically determined using transient absorption (TA) spectroscopy, Mn-TBAPy-NT exhibits a long-lived internal charge-separated (ICS) state (255.6 ns), longer than that for Mn-TBAPy-SC (4.6 ns) and a feature apparently responsible for its over 30-fold promoted hydrogen evolution with a rate of 203.5 μmol h<small>⁻¹</small> (<em>ca.</em> 10.2 mmol h<small>⁻¹</small> g<small>_cat</small><small>⁻¹</small>) under visible light and a benchmark apparent quantum efficiency (AQE), of 11.7% at 420 ± 10 nm, among MOF-type photocatalysts. Our results open a new avenue for developing highly efficient MOF-based photocatalysts.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-01-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d4ey00007b?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139648954","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":"Tunable product selectivity on demand: a mechanism-guided Lewis acid co-catalyst for CO2 electroreduction to ethylene glycol†","authors":"Yifei Li, Karin U. D. Calvinho, Mahak Dhiman, Anders B. Laursen, Hengfei Gu, Dominick Santorelli, Zachary Clifford and G. Charles Dismukes","doi":"10.1039/D3EY00237C","DOIUrl":"10.1039/D3EY00237C","url":null,"abstract":"<p >Bioinspired nickel phosphide electrocatalysts can produce more complex multi-carbon products than natural photosynthetic enzymes but controlling C-product selectivity and suppressing H<small>₂</small> evolution remain open challenges. Here, we report a significant shift in the CO<small>₂</small>RR product distribution on Ni<small>₂</small>P in the presence of boric acid/borate, a soluble Lewis acid/base co-catalyst. Using Ni<small>₂</small>P without a co-catalyst, CO<small>₂</small> reduction produces a mixture of methyl glyoxal (C<small>₃</small>) &gt; 2,3-furnadiol (C<small>₄</small>) and formic acid (C<small>₁</small>) with 100% Faradaic efficiency for carbon products. Addition of boric acid/borate shifts product selectivity to ethylene glycol (EG) with an 85% CO<small>₂</small>-Faradaic efficiency (at 10 mM, 0 V <em>vs.</em> RHE), with the balance being the aforementioned C<small>₁</small>, C<small>₃</small> and C<small>₄</small> products. The mechanism of EG formation is proposed to occur by the co-catalyst activating a reaction between surface *hydride and *glycolaldehyde on Ni<small>₂</small>P, while suppressing the aldol C–C coupling reaction that forms the C<small>₃</small> and C<small>₄</small> products. The formation of an intermediate borate-EG-diester, [(OCH<small>₂</small>CHO)<small>₂</small>B]<small>⁻</small>, is detected by <small>¹¹</small>B-NMR, which hydrolyzes to release the EG product. Extended electrolysis of boric acid modifies the surface of Ni<small>₂</small>P by forming *BO<small>₃</small>–Ni<small>₂</small>P, as shown by XPS. CO<small>₂</small> electro-reduction on *BO<small>₃</small>–Ni<small>₂</small>P in the absence of free boric acid produces exclusively ethylene oxide (EO), which slowly hydrolyzes to EG in the bicarbonate electrolyte. The combined Faradaic efficiencies for CO<small>₂</small>RR products EO + EG with free boric acid as the co-catalyst and *BO<small>₃</small>–Ni<small>₂</small>P as the cathode reaches 88% (at 0 V <em>vs</em>. RHE), a record carbon selectivity. This work illustrates the feasibility of using Lewis acid/base co-catalysts to change the established chemical reaction mechanism of an electrocatalyst to form a new, chemically predictable, more valuable product in high yield.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-01-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d3ey00237c?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139579112","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":"Photothermal catalytic oxidation of toluene over the Pt–Mn2O3/CN nanocomposite catalyst†","authors":"Xiao Yu, Chuang Zhao, Lixia Yang, Jian Zhang and Chunlin Chen","doi":"10.1039/D3EY00298E","DOIUrl":"10.1039/D3EY00298E","url":null,"abstract":"<p >The Pt–Mn<small>₂</small>O<small>₃</small>/CN catalyst formed through synthesis <em>via</em> a solvent-thermal method involves a synergistic combination of polymer CN and Pt nanoparticles loaded on Mn<small>₂</small>O<small>₃</small> to catalyze the degradation of toluene. The composition incorporates Mn<small>₂</small>O<small>₃</small> as the central element for photothermal conversion, CN as a uniformly dispersed matrix for Pt nanoparticles, and Pt as the catalytically active center, demonstrating significant efficacy. Particularly noteworthy is the discernible enhancement in the photothermal catalytic degradation capability of the Pt–Mn<small>₂</small>O<small>₃</small>/CN composite catalyst, specifically in the context of toluene. When subjected to light intensity of 300 mW cm<small>⁻²</small> and a toluene concentration of 400 ppm, Pt–Mn<small>₂</small>O<small>₃</small>/CN achieves toluene conversion and CO<small>₂</small> mineralization rates of 99% and 80.9%, respectively. This improvement primarily stems from the Pt nanoparticles inducing a substantial presence of oxygen vacancies within the catalyst structure, thereby increasing the oxygen adsorption capacity and surface mobility. This, in turn, activates adsorbed oxygen species at the catalyst's interface. The adept utilization and conversion of solar irradiance for volatile organic compound (VOC) abatement underscore its potential as an environmentally friendly and renewable energy source.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d3ey00298e?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139518493","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 minireview on electrochemical CO2 conversion based on carbonate/bicarbonate media","authors":"Tiehuai Li and Minhua Shao","doi":"10.1039/D3EY00287J","DOIUrl":"10.1039/D3EY00287J","url":null,"abstract":"<p >Direct electrochemical CO<small>₂</small> conversion in carbonate/bicarbonate based CO<small>₂</small> capture media has emerged as a promising technology for integrating carbon capture and CO<small>₂</small> electroreduction processes in recent years, garnering significant attention from researchers owing to its high energy efficiency and carbon efficiency. For a holistic understanding of the development status of this field, this minireview summarizes a series of studies on the mechanism of carbonate/bicarbonate electrolyzers. Detailed mechanisms of the electrochemical conversion of carbonate/bicarbonate, the evolution of electrolyzers, and factors influencing the performance of electrolyzers are introduced. A summary of carbonate/bicarbonate electrolyzers' performance is also provided. Representative systems and materials for regulating the selectivity towards various products (<em>e.g.</em>, CO, formate, methane, ethylene, and ethanol) and the cell voltage are highlighted. Furthermore, the challenges and future opportunities in this research area are also discussed.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-01-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d3ey00287j?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139501622","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}