EES catalysis最新文献

{"title":"Photocatalytic inactivation technologies for bioaerosols: advances and perspective","authors":"Linghui Peng, Haiyu Wang, Yuelong Wang, Guiying Li and Taicheng An","doi":"10.1039/D3EY00179B","DOIUrl":"10.1039/D3EY00179B","url":null,"abstract":"<p >Bioaerosol control systems are urgently needed to inactivate airborne pathogenic microorganisms to prevent secondary contamination. Recently, with an increasing number of studies on the characteristics of bioaerosols, researchers have gained a better understanding of bioaerosols, which has promoted the development of bioaerosol control technology. Bioaerosol photocatalytic inactivation technology shows its superiority through excellent oxidation capacity, environmental friendliness, the absence of secondary contaminations, and good compatibility. However, there are very few available studies that comprehensively summarize and present the state of bioaerosol photocatalytic inactivation technology. This article mainly reviews the recent advances in advanced materials, combined technologies, carriers and reactors, applications and performance evaluations of photocatalytic inactivation technology. The efficiency, advantages and disadvantages of these factors are comprehensively discussed. This review also highlights the practical applications, addresses the challenges, and provides a perspective on bioaerosol photocatalytic inactivation for future research.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d3ey00179b?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138519305","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":"Reaction microenvironment control in membrane electrode assemblies for CO2 electrolysis","authors":"Chuanchuan Yan, Dunfeng Gao, Juan-Jesús Velasco-Vélez and Guoxiong Wang","doi":"10.1039/D3EY00155E","DOIUrl":"10.1039/D3EY00155E","url":null,"abstract":"<p >CO<small>₂</small> electrolysis is an emerging and promising carbon neutrality technology, but currently suffers from challenging selectivity issues at industrially relevant reaction rates. Selectivity control in CO<small>₂</small> electrolysis relies on the molecular understanding and manipulation of multiple parallel reaction pathways that are equally governed by catalytically active sites and the reaction microenvironments in their vicinity. In this perspective, we summarize and discuss the latest achievements in reaction microenvironment control for active, selective, energy- and carbon-efficient CO<small>₂</small> electrolysis, with particular attention being paid to that in membrane electrode assembly electrolyzers operating at industrial current densities (≥200 mA cm<small>⁻²</small>). The effects and underlying catalytic mechanisms of reaction microenvironments tailored by functional organic molecules/polymers and reactant feed compositions on the activity and selectivity of CO<small>₂</small> electrolysis are discussed using selected examples. The efforts made to tailor acidic reaction microenvironments by controlling the transport of reactive species for carbon-efficient CO<small>₂</small> electrolysis are also exemplified. Finally, we illustrate current challenges and future opportunities in the mechanistic understanding and rational design of reaction microenvironments for improving CO<small>₂</small> electrolysis performance.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d3ey00155e?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135181739","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":"Emerging on-chip microcells in electrocatalysis: functions of window and circuit","authors":"Jinbo Wang, Mengyi Qiu, Yubin Jiang, Hang Xia, Xiuyun An, Shuangyin Wang and Yongmin He","doi":"10.1039/D3EY00168G","DOIUrl":"https://doi.org/10.1039/D3EY00168G","url":null,"abstract":"<p >An electrocatalytic process that efficiently converts the reactants into high-value-added chemicals has attracted increasing attention in renewable energy fields. Specifically, understanding such a process at a single-material level will be of fundamental importance for catalyst design and mechanism explorations as well. Thanks to the development of electronic devices, on-chip microcells have emerged as a powerful platform through which significant progress has been impressively made. Here, this review provides an overview of the progress based on on-chip microcells. We first introduce how the on-chip microcell develops from electronic transistors like field effect-based and electric double-layer-based ones. Next, we discuss current achievements relying on their two basic functions: the reaction window and the circuit; the former is mainly focused on the active sites, for example, identification of active sites as well as monitoring of their changes; the latter sheds light on its circuit characteristics, such as electrical-field modulation, contact engineering for charge injection, and <em>in situ</em> conductance measurement of metallic and nonmetallic catalysts. Finally, we give personal perspectives on this emerging field, including the current challenges and potential applications.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"71906550","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":"Atomically imaging single atom catalysts and their behaviors by scanning tunneling microscopy","authors":"Hongli Sun, Like Sun, Yanglong Liao, Zirui Zhou, Jie Ding, Shaotang Song, Bin Liu and Chenliang Su","doi":"10.1039/D3EY00174A","DOIUrl":"10.1039/D3EY00174A","url":null,"abstract":"<p >Understanding the mechanism of single-atom catalysis is essential to design and refine systems for improved catalytic performance. However, given the complex structure and large variety of single-atom catalysts (SACs), characterizing the single-atom catalytically active sites is extremely tricky and challenging. Over the past decade, although still far from satisfactory, scanning tunneling microscopy (STM) has helped provide numerous fundamental insights to understand single-atom catalysis. In this review, we summarize how STM enables atomically precise imaging of SACs including their geometric and electronic structures and their behaviors in the activation of absorbed small molecules, and how the combination of STM and other techniques helps to reveal charge states, charge transfers, dynamic reaction processes, and reaction mechanisms in single-atom catalysis. Finally, the future expectations on STM in three-dimensional, spatial and temporal imaging, and <em>operando</em> characterization are proposed. We believe that the combination of STM and single-atom catalysis is attractive and will further flourish heterogeneous catalysis research.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"57970020","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":"Advances and challenges in scalable carbon dioxide electrolysis","authors":"Ji Wei Sun, Huai Qin Fu, Peng Fei Liu, Aiping Chen, Porun Liu, Hua Gui Yang and Huijun Zhao","doi":"10.1039/D3EY00159H","DOIUrl":"10.1039/D3EY00159H","url":null,"abstract":"<p >The electrochemical CO<small>₂</small> reduction reaction (CO<small>₂</small>RR) is an effective way of utilizing carbon and can be economically profitable by converting captured CO<small>₂</small> into valuable products. In the last decade, significant research efforts have been dedicated to CO<small>₂</small>RR technology and significant breakthroughs in materials design, mechanistic understanding and device applications have been made. Although laboratory-level CO<small>₂</small>RR performance has shown its potential prospects, scalable CO<small>₂</small> electrolysis is still far from market ready. The keys for industrialization are to cut running costs, increase the CO<small>₂</small> conversion rate and obtain high industrial value reaction products. Here, we start by systematically introducing the current research progress made in CO<small>₂</small> electrolyzer development in terms of the device structure and reaction environments. Then, the current problems in the scale-up process and corresponding solutions are summarized. Some improvement strategies and development directions are proposed, for example, cathodic salting, the use of ion exchange membranes and flow channel design. This perspective illustrates the importance of practical electrolyzers, which will guide the design of scalable CO<small>₂</small> electrolyzers and accelerate the commercialization process of CO<small>₂</small>RR technology.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"57969621","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":"Reducing the pH dependence of hydrogen evolution kinetics via surface reactivity diversity in medium-entropy alloys†","authors":"Bao Zhang, Jia Yao, Jia Liu, Tao Zhang, Houzhao Wan and Hao Wang","doi":"10.1039/D3EY00157A","DOIUrl":"10.1039/D3EY00157A","url":null,"abstract":"<p >The water dissociation step of the hydrogen evolution reaction is a well-known pH-dependent process, which makes sustainable hydrogen production suffer from sluggish kinetics. Herein, we demonstrate a surface reactivity diversity approach to reduce the pH dependence of HER kinetics in medium-entropy alloys. Grand canonical potential based calculation, CO-oxidation and potential of zero charge results showed that shifts in the Fermi level in neutral electrolytes lead to stronger M–H bonding (M = Ni, Pt, <em>etc.</em>) compared to those in basic solutions. These pH-dependent binding energies disrupt the optimized adsorption strength of advanced alkaline HER catalysts. By introducing a combination of a high surface reactivity metal (Mo) and a low surface reactivity metal (Cu/Zn) into Ni alloys, this surface reactivity diversity approach can significantly accelerate HER kinetics and allows for favorable adsorption of hydrogen and hydroxyl species at different pH levels. The resulting NiCuMo medium-entropy alloy exhibited impressive HER performance, with an overpotential of 63 mV at a current density of 100 mA cm<small>⁻²</small> in alkaline electrolyte and 115 mV in neutral electrolyte. The intrinsic neutral HER activity of this NiCuMo is 3.65 times that of the benchmark alkaline HER catalyst. Furthermore, the NiCuMo-based membrane electrode assembly water electrolyzer can be stably operated for at least 200 h at a larger current density of 1.5 A cm<small>⁻²</small>. This surface reactivity diversity approach presents a promising design framework for less pH-dependent electrocatalysis.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"57969597","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":"Enhancing C≥2 product selectivity in electrochemical CO2 reduction by controlling the microstructure of gas diffusion electrodes†","authors":"Francesco Bernasconi, Alessandro Senocrate, Peter Kraus and Corsin Battaglia","doi":"10.1039/D3EY00140G","DOIUrl":"10.1039/D3EY00140G","url":null,"abstract":"<p >We fabricate polymer-based gas diffusion electrodes with controllable microstructure for the electrochemical reduction of CO<small>₂</small>, by means of electrospinning and physical vapor deposition. We show that the microstructure of the electrospun substrate is affecting the selectivity of a Cu catalyst, steering it from H<small>₂</small> to C<small>₂</small>H<small>₄</small> and other multicarbon products. Specifically, we demonstrate that gas diffusion electrodes with small pores (<em>e.g.</em> mean pore size 0.2 μm) and strong hydrophobicity (<em>e.g.</em> water entry pressure &gt;1 bar) are necessary for achieving a remarkable faradaic efficiency of ∼50% for C<small>₂</small>H<small>₄</small> and ∼75% for C<small>_≥2</small> products in neutral 1M KCl electrolyte at 200 mA cm<small>⁻²</small>. We observe a gradual shift from C<small>₂</small>H<small>₄</small> to CH<small>₄</small> to H<small>₂</small> during long-term electrochemical reduction of CO<small>₂</small>, which we ascribe to hygroscopic carbonate precipitation in the gas diffusion electrode resulting in flooding of the Cu catalyst by the electrolyte. We demonstrate that even with minimal electrolyte overpressure of 50 mbar, gas diffusion electrodes with large pores (mean pore size 1.1 μm) lose selectivity to carbon products completely, suddenly, and irreversibly in favor of H<small>₂</small>. In contrast, we find that gas diffusion electrodes with small pore size (mean pore size 0.2 μm) and strong hydrophobicity (water entry pressure ∼5 bar) are capable of resisting up to 1 bar of electrolyte overpressure during CO<small>₂</small>RR without loss of selectivity. We rationalize these experimental results in the context of a double phase boundary reactivity, where an electrolyte layer covers the Cu catalyst and thus governs local CO<small>₂</small> availability. Our results emphasize the pivotal role of microstructure and hydrophobicity in promoting high C<small>_≥2</small> product selectivity and long-term stability in CO<small>₂</small>RR flow cells.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-08-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"57969276","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":"Electroreforming injects a new life into solid waste","authors":"Yingxin Ma, Yu Zhang, Wenfang Yuan, Mengmeng Du, Sailei Kang and Bocheng Qiu","doi":"10.1039/D3EY00147D","DOIUrl":"https://doi.org/10.1039/D3EY00147D","url":null,"abstract":"<p >The drive to upgrade the system capacity for renewable electricity, coupled with relieving our reliance on the finite fossil resources, promotes the exploration for economically competitive and environmentally friendly technologies that can steer the conversion of the renewable feedstocks into fuels, chemicals, and materials. An appealing remedy is to utilize ubiquitous solid waste (<em>e.g.</em>, biomass and plastics) as platform precursors to synthesize valuable chemicals used globally on a daily basis. Although the defined functionality of biomass differs from that of plastics, they share considerable structural similarities in terms of the polymeric nature and the type of bonds connecting the constituent monomers, thereby establishing an intimate correlation between their valorization routes. Electroreforming methodology towards upgrading of biomass and plastic wastes into commodity chemicals coupled with hydrogen evolution is thus viable and meanwhile remains intriguing. In this review, we draw parallels between electrochemical valorization of biomass and plastics, with a focus on elucidating the state-of-the-art catalysts for each documented reaction and evaluating their corresponding techno-economy. In parallel, the pretreatment methodologies for raw solid waste and the progress in computational simulations and <em>operando</em> spectroscopies are reviewed in detail. We conclude with a comprehensive discussion of the emerging challenges for catalyst and reactor optimization, large-scale operation, and technology flexibility and compatibility.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-08-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"71906551","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":"The more the better: on the formation of single-phase high entropy alloy nanoparticles as catalysts for the oxygen reduction reaction†","authors":"Rebecca K. Pittkowski, Christian M. Clausen, Qinyi Chen, Dragos Stoian, Wouter van Beek, Jan Bucher, Rahel L. Welten, Nicolas Schlegel, Jette K. Mathiesen, Tobias M. Nielsen, Jia Du, Asger W. Rosenkranz, Espen D. Bøjesen, Jan Rossmeisl, Kirsten M. Ø. Jensen and Matthias Arenz","doi":"10.1039/D3EY00201B","DOIUrl":"10.1039/D3EY00201B","url":null,"abstract":"<p >High entropy alloys (HEAs) are an important new material class with significant application potential in catalysis and electrocatalysis. The entropy-driven formation of HEA materials requires high temperatures and controlled cooling rates. However, catalysts in general also require highly dispersed materials, <em>i.e.</em>, nanoparticles. Only then a favorable utilization of the expensive raw materials can be achieved. Several recently reported HEA nanoparticle synthesis strategies, therefore, avoid the high-temperature regime to prevent particle growth. In our work, we investigate a system of five noble metal single-source precursors with superior catalytic activity for the oxygen reduction reaction. Combining <em>in situ</em> X-ray powder diffraction with multi-edge X-ray absorption spectroscopy, we address the fundamental question of how single-phase HEA nanoparticles can form at low temperatures. It is demonstrated that the formation of HEA nanoparticles is governed by stochastic principles and the inhibition of precursor mobility during the formation process favors the formation of a single phase. The proposed formation principle is supported by simulations of the nanoparticle formation in a randomized process, rationalizing the experimentally found differences between two-element and multi-element metal precursor mixtures.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-08-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"57969881","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":"Copper-based catalysts for CO2 hydrogenation: a perspective on active sites","authors":"Yun-Fei Shi, Sicong Ma and Zhi-Pan Liu","doi":"10.1039/D3EY00152K","DOIUrl":"https://doi.org/10.1039/D3EY00152K","url":null,"abstract":"<p >CO<small>₂</small> hydrogenation is regarded as a revolutionized field in heterogeneous catalysis, not only mitigating environmental problems caused by greenhouse gases but also producing valuable chemicals. This Perspective, going over both theoretical and experimental advances, aims to bridge Cu-based catalyst structures, the most important type of CO<small>₂</small> hydrogenation catalyst, and their catalysis applications with varied activity and selectivity. We provide a systematic overview of the catalytic active sites, the reaction mechanism, and their impact on the reaction selectivity, stability, and activity for CO<small>₂</small> hydrogenation. There is a particular focus on the nature of the industrial Cu/ZnO/Al<small>₂</small>O<small>₃</small> catalyst, where a large volume of literature is available exploring the reaction energetics on the possible reaction sites, including Cu metal, CuZn alloy, and ZnO<small>_<em>x</em></small>H<small>_<em>y</em></small> overlayers. The recent advances in designing better catalytic active sites, such as the Cu single-atom catalyst, supported Cu cluster catalyst, and bimetallic Cu–M, are then followed to illustrate how the activity and selectivity vary upon changing the active sites. Our perspectives on the future research directions are finally provided, which should benefit the understanding of complex catalytic active sites and the design of better CO<small>₂</small> hydrogenation catalysts.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"71906552","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}