EES catalysis最新文献

{"title":"Research progress and perspectives on photocatalysts based on the lead-free double halide perovskite","authors":"Do Yeon Heo, Mahider Asmare Tekalgne and Soo Young Kim","doi":"10.1039/D3EY00229B","DOIUrl":"10.1039/D3EY00229B","url":null,"abstract":"<p >Photocatalytic technology stands as a promising solution to address the current energy and environmental challenges. Halide perovskites, particularly lead-free double halide perovskites, have garnered recognition as next-generation photocatalysts due to their adjustable bandgap, low binding energy, broad visible light absorption range, and efficient charge carrier transfer. In this review, we explore the utilization of lead-free double halide perovskites characterized by their non-toxic attributes and diverse chemical compositions and properties as photocatalysts for both hydrogen production and carbon dioxide reduction. We commence by presenting an overview of lead-free double halide perovskites, followed by a comprehensive analysis of recent research outcomes pertaining to their application as photocatalysts for hydrogen production and carbon dioxide reduction. Lastly, we discuss the challenges and prospects associated with lead-free double halide perovskite photocatalysts. This review is anticipated to serve as a valuable reference for the development of lead-free double halide perovskite-based photocatalysts, addressing critical aspects in the pursuit of achieving high-efficiency hydrogen generation and carbon dioxide reduction, crucial for our future energy and environmental needs.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 1","pages":" 94-108"},"PeriodicalIF":0.0,"publicationDate":"2023-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d3ey00229b?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135152839","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":"Harnessing single-atom catalysts for CO2 electroreduction: a review of recent advances","authors":"Chang Chen, Jiazhan Li, Xin Tan, Yu Zhang, Yifan Li, Chang He, Zhiyuan Xu, Chao Zhang and Chen Chen","doi":"10.1039/D3EY00150D","DOIUrl":"10.1039/D3EY00150D","url":null,"abstract":"<p >Electrochemical CO<small>₂</small> reduction is an effective pathway to convert CO<small>₂</small> into valuable fuels and chemicals, which provides a potential alternative to fossil fuel resources and plays a notable role in mitigating environmental issues and energy crises. The feasibility of the CO<small>₂</small> reduction reaction (CO<small>₂</small>RR) hinges on the development of catalysts that feature high activity, selectivity, and stability. As a new research frontier, single-atom catalysts (SACs) have shown immense potential in the field of CO<small>₂</small> reduction by virtue of their unique geometric/electronic structures, and have also provided new opportunities for atomic-level understanding of structure–function relationships. Therefore, this review aims to outline recent advances of SACs for CO<small>₂</small>RR. We start by introducing the current research status and general synthesis strategies of SACs, and then shift our focus to analyzing the various regulation strategies and deciphering the structure–function relationships of SACs in the CO<small>₂</small>RR. Finally, we propose future directions and opportunities for CO<small>₂</small>RR-oriented SACs, while also highlighting potential challenges that may be encountered along the way.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 1","pages":" 71-93"},"PeriodicalIF":0.0,"publicationDate":"2023-10-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d3ey00150d?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"136304871","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":"Boosting the catalytic performance of metal–zeolite catalysts in the hydrocracking of polyolefin wastes by optimizing the nanoscale proximity†","authors":"Xinlei Han, Xinru Zhou, Tuo Ji, Feng Zeng, Weiping Deng, Zhenchen Tang and Rizhi Chen","doi":"10.1039/D3EY00180F","DOIUrl":"10.1039/D3EY00180F","url":null,"abstract":"<p >Hydrocracking polyolefins using bifunctional metal–zeolite catalysts is a pivotal strategy for the catalytic upcycling of plastic waste to produce value-added fuels. However, the macro-molecular size and stable C–C bond of polyolefins impose major challenges on catalyst design based on noble metal and microporous zeolites. The lack of investigation into the nanoscale proximity between Pt and USY has hindered the development of an evolving generation of catalysts. Herein, we report Pt/USY prepared by colloid-immobilization method with Pt nanoparticles exclusively located on the surface of USY is a superior catalyst (&gt;50% higher activity) compared to its analogues that have Pt inside or away from USY crystalline, reaching a selectivity to gasoline (C<small>_5–12</small>) over 90%. The formation rate of liquid products reaches 6122 g<small>_liquid</small> g<small>_Pt</small><small>⁻¹</small> h<small>⁻¹</small> and 5048 g<small>_liquid</small> g<small>_Pt</small><small>⁻¹</small> h<small>⁻¹</small> in hydrocracking polyethylene (PE) and polypropylene (PP) at 280 °C, respectively. The hydrocracking of model alkanes with different molecular sizes demonstrates the nanoscale Pt-USY proximity as a key criterion in optimizing the accessibility and acidic environment of Pt, and the diffusion distance between metal and acid sites. These findings comprise a significant step forward toward rational catalyst design aiming at upcycling plastic waste for sustainable fuel production.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 1","pages":" 300-310"},"PeriodicalIF":0.0,"publicationDate":"2023-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d3ey00180f?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"136202105","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":"Highly selective Ag foam gas diffusion electrodes for CO2 electroreduction by pulsed hydrogen bubble templation†","authors":"Hendrik Hoffmann, Maximilian Kutter, Jens Osiewacz, Melanie-Cornelia Paulisch-Rinke, Steffen Lechner, Barbara Ellendorff, Annika Hilgert, Ingo Manke, Thomas Turek and Christina Roth","doi":"10.1039/D3EY00220A","DOIUrl":"10.1039/D3EY00220A","url":null,"abstract":"<p >The electrochemical reduction of carbon dioxide to valuable fossil-free products opens up a way to close the carbon cycle, if based solely on renewable energy sources. Making the process industrially viable, however, needs high CO<small>₂</small> conversion rates, efficient electrodes, and high selectivity for desired products. To reach this goal, highly catalytically active porous electrodes with maximized surface areas are required. We combined pulsed electrochemical deposition of the Ag foam catalyst with ionomer infiltration of the electrode to produce Ag-based gas diffusion electrodes (GDEs) in a facile and fast production process. Using the dynamic hydrogen bubble templation method (DHBT), we utilized the parasitic hydrogen evolution reaction (HER) to aid the solvent free structuring of the 3D catalyst network and directly manufacture a GDE. Different deposition parameters and in particular pulse-to-pause ratios increased the amount of deposited catalyst and successfully reduced the overpotential during CO<small>₂</small>RR operation. To inhibit electrode flooding and decrease CO<small>₂</small> mass transport limitations during CO<small>₂</small>RR, we further infiltrated the electrode with a suitable perfluorosulfonic acid ionomer. SEM and EDS analyses showed a homogeneous Ag/F distribution along the cross section of the electrodes. These electrodes catalyzed the conversion of CO<small>₂</small> to CO at industrially viable current densities of 500 mA cm<small>⁻²</small> with an unprecedented faradaic efficiency up to 76% in 1 M KHCO<small>₃</small>.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 1","pages":" 286-299"},"PeriodicalIF":0.0,"publicationDate":"2023-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d3ey00220a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138519295","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":"Single atom catalysts for water electrolysis: from catalyst-coated substrate to catalyst-coated membrane","authors":"Sol A Lee, Sang Eon Jun, Sun Hwa Park, Ki Chang Kwon, Jong Hun Kang, Min Sang Kwon and Ho Won Jang","doi":"10.1039/D3EY00165B","DOIUrl":"10.1039/D3EY00165B","url":null,"abstract":"<p >Green hydrogen production through water electrolysis is considered the next-generation technology capable of industrial-scale hydrogen production to achieve carbon neutrality. The core of constructing a water electrolyzer lies in designing the membrane electrode assembly (MEA) with optimal integration of the membrane, electrocatalysts, and gas diffusion layer. Among the two representative MEA fabrication methods, catalyst-coated substrates (CCS) and catalyst-coated membranes (CCM), CCM shows great promise due to its catalyst layer/membrane interface contact and scalability. The key factor in the CCM method is the effective application of the powdered catalyst onto the membrane. In this respect, the utilization of single-atom catalysts (SACs) has emerged as a noteworthy focus due to their unprecedented catalytic activity resulting from unique electronic/atomic configurations and high atomic utilization efficiency. Incorporating SACs into CCM–MEA has the potential to be a cutting-edge water electrolysis technology. However, it is still in its infancy due to the instability of the components (SACs, membranes, ionomers, supports) and degradation during the SACs–CCM–MEA fabrication and cell operation. Herein, we outline the representative fabrication method of MEA and provide a comprehensive analysis of SACs applicable to MEA. Then, we discuss the advantages of SACs–CCM–MEA and the challenges for industrial hydrogen production. Finally, this review concludes with future perspectives on the development of single-atom catalyst-coated membranes and the expected achievements.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 1","pages":" 49-70"},"PeriodicalIF":0.0,"publicationDate":"2023-10-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d3ey00165b?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138519294","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":"Gas-phase errors in computational electrocatalysis: a review","authors":"Ricardo Urrego-Ortiz, Santiago Builes, Francesc Illas and Federico Calle-Vallejo","doi":"10.1039/D3EY00126A","DOIUrl":"10.1039/D3EY00126A","url":null,"abstract":"<p >Currently, computational models based on density functional theory (DFT) are intensively used for the analysis of electrocatalytic reactions and the design of enhanced catalysts. As the accuracy of these models is subjected to the quality of the input data, knowing the intrinsic limitations of DFT is crucial to improve computational predictions. A common pitfall of DFT is the estimation of the total energies of molecules, particularly those containing double and triple bonds. In this review, we show how gas-phase errors permeate thermodynamic and kinetic models of customary use in electrocatalysis, potentially compromising their predictiveness. First, we illustrate how these errors can be identified and provide a list of corrections for common molecules and functional groups. Subsequently, we explain how the errors spread from simple reaction energy calculations to adsorption energies, scaling relations, equilibrium potentials, overpotentials, and Sabatier-type activity plots. Finally, we list the remaining challenges toward an improved assessment of energetics at solid–gas–liquid interfaces.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 1","pages":" 157-179"},"PeriodicalIF":0.0,"publicationDate":"2023-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d3ey00126a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138519306","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":"Structural engineering of catalysts for ammonia electrosynthesis from nitrate: recent advances and challenges","authors":"Wenxi Qiu, Yuanting Liu, Minghao Xie, Zhaoyu Jin, Panpan Li and Guihua Yu","doi":"10.1039/D3EY00184A","DOIUrl":"10.1039/D3EY00184A","url":null,"abstract":"<p >Ammonia (NH<small>₃</small>) is an indispensable industrial chemical used in fertilizer production and energy carriers. However, its production through the Haber–Bosch process requires high temperature and high pressure, consuming significant energy and releasing large amounts of CO<small>₂</small>, rendering it unsustainable. As a result, sustainable approaches for ammonia synthesis powered by renewable electricity have gained significant attention, such as the electrocatalytic N<small>₂</small> reduction reaction (N<small>₂</small>RR) and nitrate reduction reaction (NitRR). This review summarizes recent advancements in the design strategies of electrocatalysts for the NitRR, highlighting synthetic methods such as doping, alloying, single-atom engineering, nanoconfinement, size-regulation, and tandem catalysis. These strategies aim to tune the adsorption of reactants and intermediates or enhance proton–electron transfer. Future studies could explore new electrocatalysts for efficient NitRR based on the strategies summarized in this review to improve nitrate pollution removal efficiency and ammonia production rates. Furthermore, the challenging questions raised at the end of the paper, such as optimizing the reaction kinetics of the NitRR and improving catalyst selectivity and stability, can provide new directions and insights for future catalyst design.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 1","pages":" 202-219"},"PeriodicalIF":0.0,"publicationDate":"2023-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d3ey00184a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138519308","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 chemist's guide to photoelectrode development for water splitting – the importance of molecular precursor design","authors":"Thom R. Harris-Lee, Frank Marken, Cameron L. Bentley, Jie Zhang and Andrew L. Johnson","doi":"10.1039/D3EY00176H","DOIUrl":"https://doi.org/10.1039/D3EY00176H","url":null,"abstract":"<p >Photoelectrochemical (PEC) water splitting is a promising method for generating green hydrogen as a solar fuel, overcoming the issues associated with unreliability and periodicity of renewable technologies. While research in this field is growing, there is a distinct gap between complex device development and fundamental synthesis of the individual materials. For optimal device fabrication we need materials scientists and engineers to create complex multicomponent photoelectrodes, but also inorganic chemists to design bespoke precursors tailored to produce highly efficient, specifically designed photoelectrode materials. The success of precursor design for semiconductors in fields such as microelectronics has proven the significant impact of the precursor, however, this approach has yet to be used extensively in device fabrication for PEC water splitting. This review acts as a guide towards bespoke precursor development for the fabrication of tailored thin films; particularly how to design the structure and composition of the precursor to promote and enhance the most desired properties, including solubility, volatility, and thermal decomposition. The key areas of focus for device design are outlined, including both single thin film performance and overall device modifications and additions to create a high-performance PEC water splitting electrode. There is a specific emphasis towards chemical vapour deposition techniques due to the suitability for scale-up and commercial application compared to alternatives, and importantly, the significant influence of the molecular precursor on the deposition, and hence its link to synthetic chemistry. We aim to direct more synthetic chemists towards the field of PEC water splitting, encouraging collaboration to connect these two areas and bring the target of a commercially and industrially viable PEC system ever closer.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 6","pages":" 832-873"},"PeriodicalIF":0.0,"publicationDate":"2023-09-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"71906549","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Elucidating the validity of electronic characteristics of transition metal perovskites as descriptors bridging electro- and chemocatalysis†","authors":"Sonja D. Mürtz, Johannes Simböck, Feng Zeng, Mahnaz Ghiasi, Simon Schönebaum, Ulrich Simon, Frank M. F. de Groot and Regina Palkovits","doi":"10.1039/D3EY00206C","DOIUrl":"https://doi.org/10.1039/D3EY00206C","url":null,"abstract":"<p >The analysis of electronic characteristics as descriptors for the efficacy of catalysts provides fundamental insights into catalyst design criteria, but few studies address the applicability of descriptors across a broader range of reactions. This study on perovskite-type, B-site substituted LaCoO<small>₃</small> derivates analyses the generalisability of the descriptor nature of electronic characteristics for electro- and chemocatalytic reactions – more specifically the occupancy of transition metal (TM) 3d orbitals, charge-transfer energy (CTE), and covalency in the interaction of O 2p – TM 3d states. The results show that among the analysed characteristics only covalency is a quasi-linear descriptor for the performance in electrocatalytic oxygen evolution reaction (OER), glycerol electro-oxidation reaction (GOR), as well as in five chemocatalytic reactions. The analysis of the reduction reaction of NO or N<small>₂</small>O by CO illustrates that not only reaction rates but also selectivity is determined by the same electronic catalyst characteristics. Measurement conditions in the analysis of electronic characteristics need to be chosen to recreate the oxidation state during the reaction-specific kinetically relevant step to yield adequate descriptor correlations. The results imply that significant synergies may be leveraged by enhanced collaboration across electro- and chemocatalysis research.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 6","pages":" 961-971"},"PeriodicalIF":0.0,"publicationDate":"2023-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"71906922","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Recent advances in tunable metal–support interactions for enhancing the photocatalytic nitrogen reduction reaction","authors":"Bing-Hao Wang, Guang-Hui Chen, Biao Hu, Lang Chen, Xiong Wang, Sheng Tian, Xing-Sheng Hu, Yang Li, Chao Peng and Shuang-Feng Yin","doi":"10.1039/D3EY00191A","DOIUrl":"10.1039/D3EY00191A","url":null,"abstract":"<p >Ammonia (NH<small>₃</small>), as an important foundational chemical and green hydrogen energy carrier, plays an indispensable role in the development of human society. However, it is evident that the traditional process for NH<small>₃</small> synthesis is no longer in line with the times due to its drawbacks, such as high energy consumption and high carbon emission. In recent years, the photocatalytic nitrogen reduction reaction (PNRR), which reduces N<small>₂</small> to NH<small>₃</small> under mild conditions using inexhaustible solar energy, has been considered as a promising alternative. Nevertheless, the catalytic efficiency of the PNRR is low and far from realizing practical applications owing to the weak N<small>₂</small> adsorption, hard dissociation of inert N<img>N, and competing reactions of hydrogen precipitation. Metal–support interactions (MSIs) provide an efficient way to adjust the performance of both the active metal and support in the photocatalytic process through geometric, electronic and bifunctional effects. The design of heterogeneous photocatalysts with tunable MSIs has been proved to be a feasible way to enhance their catalytic performance for the PNRR. In this review, we summarize the recent developments in MSI photocatalysts involved in nitrogen fixation. Firstly, the mechanism of MSIs and their characterization as well as the synthesis strategies for photocatalysts with MSIs are briefly outlined. Subsequently, the electronic and bifunctional effects of MSI photocatalysts and the corresponding PNRR mechanism are focused on, from the aspects of supports such as metal oxides, bismuth oxyhalides, metal sulfides, metal–organic frameworks (MOFs) and carbon nitrides. Finally, the future developments in this area such as creating state-of-the-art materials with MSIs and synthesis strategies and developing advanced techniques to investigate reaction mechanisms for N<small>₂</small> fixation are discussed. It is expected that this review can provide some guidance for understanding and rationally designing MSI photocatalysts, especially for boosting the PNRR.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 1","pages":" 180-201"},"PeriodicalIF":0.0,"publicationDate":"2023-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d3ey00191a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138519272","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}