{"title":"MXene-supported single-atom and nano catalysts for effective gas-phase hydrogenation reactions","authors":"Yilong Yan , Djibril Sall , Lola Loupias , Stéphane Célérier , Mimoun Aouine , Pascal Bargiela , Mathieu Prévot , Franck Morfin , Laurent Piccolo","doi":"10.1016/j.mtcata.2023.100010","DOIUrl":"https://doi.org/10.1016/j.mtcata.2023.100010","url":null,"abstract":"<div><p>Transition metal carbides are known as efficient catalysts or catalyst supports and two-dimensional carbides (MXenes) offer renewed possibilities to anchor metal atoms and promote catalytic performances. This paper first presents an in-depth study of the elaboration of Pt or Pd-loaded Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub> MXenes and their unstacking for gas-phase catalysis investigations, along with step-by-step characterization by XRD, XPS, SEM and STEM. In particular, the influence of the MXene preparation method (HF <em>vs</em>. LiF-HCl etchants) on surface structure/composition and metal dispersion/oxidation state is disclosed. Second, the catalytic hydrogenation performances of these materials are reported, and reveal the interest of low-loaded Pt/MXene single-atom catalysts in terms of activity, selectivity and resistance to sintering. They present an unusually high selectivity to 2-butene – without butane formation – in butadiene hydrogenation, a model reaction of applied interest for the petrochemical industry. Moreover, in CO<sub>2</sub> reduction to CO (reverse water-gas shift reaction, relevant to greenhouse-gas valorization), these catalysts exhibit up to 99 % selectivity and a superior Pt-molar activity with respect to oxide-supported references. This work may stimulate the elaboration and investigation of other MXene-based systems for thermal heterogeneous catalysis, which remains rarely addressed on these materials.</p></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"2 ","pages":"Article 100010"},"PeriodicalIF":0.0,"publicationDate":"2023-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49751443","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}
Zhishan Liang , Carmen Lee , Jiawei Liu , Yue Hu , Dongxue Han , Li Niu , Qingyu Yan
{"title":"Booming electrocatalysts for urea synthesis via nitrogen-integrated carbon dioxide reduction reaction","authors":"Zhishan Liang , Carmen Lee , Jiawei Liu , Yue Hu , Dongxue Han , Li Niu , Qingyu Yan","doi":"10.1016/j.mtcata.2023.100011","DOIUrl":"https://doi.org/10.1016/j.mtcata.2023.100011","url":null,"abstract":"<div><p>The traditional method of urea production is a carbon-emitting, energy-intensive technology that contradicts the concept of carbon neutrality. Fortunately, the use of renewable energy in electrochemical synthesis has shown great potential for producing high-value nitrogen products, making electrocatalytic urea production a promising and sustainable approach. However, the low yield and Faraday efficiency, as well as the unclear mechanism of C-N bond formation, limit its large-scale industrial development. Researchers are seeking higher-performance electrocatalysts. This article discusses in detail the latest progress in the electrochemical synthesis of urea using carbon dioxide and various nitrogen sources, including catalyst design and preparation, as well as the mechanism of C-N coupling reactions. It also provides comprehensive analysis on the challenges and prospects facing urea electro-synthesis. The development of targeted and efficient new catalysts for urea synthesis is anticipated to bring about more sustainable and cost-effective production methods.</p></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"2 ","pages":"Article 100011"},"PeriodicalIF":0.0,"publicationDate":"2023-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49727257","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}
Wei Zhang , Yu Yang , Yunxin Li , Fengwang Li , Mingchuan Luo
{"title":"Recent progress on integrated CO2 capture and electrochemical upgrading","authors":"Wei Zhang , Yu Yang , Yunxin Li , Fengwang Li , Mingchuan Luo","doi":"10.1016/j.mtcata.2023.100006","DOIUrl":"https://doi.org/10.1016/j.mtcata.2023.100006","url":null,"abstract":"<div><p>Technologies for CO<sub>2</sub> capture and utilization (CCU) are crucial for combating ever-increasing climate change. While the electrochemical conversion of captured CO<sub>2</sub> has flourished in the past few years, CO<sub>2</sub> capturing techniques are relatively mature. Typical capturing media include alkaline and amine solutions, as well as porous nanomaterials. Scaling CCU requires efficient integration of initial capture and subsequent conversion processes into one device, which is typically referred to as an integrated process. This approach has witnessed notable progress in recent years, which motivates this timely and comprehensive review. We first compare the economic aspects of separate and integrated CCU systems. Then, we discuss the separate CCU approaches that have traditionally been employed and expound on the motivations to develop an integrated system. We focus specifically on two integrated CCU approaches – direct electrolysis of capture solutions and the adoption of bifunctional porous electrodes. We also introduce the working mechanism of each approach and the latest developments, along with a comprehensive discussion on remaining challenges. To conclude, we provide an overall evaluation and outlook on advancing this integrated approach for CCU.</p></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"2 ","pages":"Article 100006"},"PeriodicalIF":0.0,"publicationDate":"2023-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49751767","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}
Yaming Hao , Xueting Cao , Can Lei , Zhe Chen , Xuejing Yang , Ming Gong
{"title":"Chemical oxygen species on electrocatalytic materials during oxygen evolution reaction","authors":"Yaming Hao , Xueting Cao , Can Lei , Zhe Chen , Xuejing Yang , Ming Gong","doi":"10.1016/j.mtcata.2023.100012","DOIUrl":"https://doi.org/10.1016/j.mtcata.2023.100012","url":null,"abstract":"<div><p>Oxygen evolution reaction (OER) is a crucial half-reaction in electrochemical water splitting, and efficient and durable electrocatalysts are required to improve the sluggish OER kinetics. However, the inevitable formation of chemical oxygen species (COSs) in the OER process heavily impacts the reaction pathway and kinetics. Precisely identifying the COSs generated during OER and acknowledging their chemo-reactivity is highly beneficial for understanding the OER mechanism and facilitating the rational design of advanced catalysts. One of the major challenges in probing the COSs is the detection of COSs under working conditions due to the transient nature and relative low coverage. This review summarizes various COSs detected on different OER electrocatalysts, including adsorbed hydroxyl (M-OH*), adsorbed oxygen (M-O*), adsorbed superoxide intermediates (M-OOH* and M-OO<sup>n-</sup>*). With these COSs probed, the possible OER mechanisms with the inter-conversion of these COSs are described. Additionally, the detailed in situ techniques for characterizing specific COSs are also introduced. Finally, we discuss remaining challenges in identifying the COSs and provide some perspectives for the design of next-generation OER electrocatalysts. By emphasizing the COSs during OER, we aim to provide vivid images of the OER transformations on the atomic scales and encourage more studies on correlating the atomic pictures of OER pathways with the active sites as well as catalyst structures.</p></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"2 ","pages":"Article 100012"},"PeriodicalIF":0.0,"publicationDate":"2023-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49727267","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 of single-atom alloy catalyst: Properties, synthetic methods and electrocatalytic applications","authors":"Jiahao Zhuang, Dingsheng Wang","doi":"10.1016/j.mtcata.2023.100009","DOIUrl":"https://doi.org/10.1016/j.mtcata.2023.100009","url":null,"abstract":"<div><p>Developing high-performance and cost-effective electrocatalysts for clean and renewable energy conversion process has been proved a promising approach to deal with the global energy and environment issues. Single-atom alloy (SAA) catalyst, with foreign metal atoms atomically dispersed in the surface of a host metal, combines the merits of conventional metal alloys and single-atom catalysts. The maximum atomic utilization of active metal and unique structural and electrical properties of SAA offer great potential in boosting electrocatalytic activity and reducing the cost of manufacture. Meanwhile, the well-defined active sites raise an opportunity to shed the light on structure-activity relationship and further direct the synthesis of high-efficiency electrocatalysts. Herein, we focus on the recent developments of advanced SAA catalysts and discussed the general properties of SAAs. Then the design principle and synthetic methods were summarized. Next, we highlighted the practical applications of SAAs in electrocatalytic energy conversion and chemicals production, including hydrogen evolution reaction, oxygen evolution reaction, CO<sub>2</sub> reduction reaction, N<sub>2</sub> reduction reaction and other representative reactions. Finally, the challenges and future directions of SAAs are presented.</p></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"2 ","pages":"Article 100009"},"PeriodicalIF":0.0,"publicationDate":"2023-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49751111","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":"Short-to-medium-range order in amorphous nanocatalysts","authors":"Geng Wu, Xiao Han, Xun Hong","doi":"10.1016/j.mtcata.2023.100025","DOIUrl":"https://doi.org/10.1016/j.mtcata.2023.100025","url":null,"abstract":"<div><p>Amorphous nanocatalysts have attracted significant attention due to their outstanding catalytic performance. Recent research has indicated that the performance of amorphous nanocatalysts is closely related to the short-to-medium-range order. This perspective aims to provide a comprehensive summary of the latest advances in understanding the significance of short-to-medium-range order in amorphous nanocatalysts and its correlation with catalytic performance. This perspective commences by presenting advanced methods employed for characterizing the short-to-medium-range order of amorphous nanocatalysts, including nanobeam electron diffraction, scanning transmission electron microscopy, atomic electron tomography, pair distribution function, and X-ray absorption fine structure spectroscopy. Next, the effect of short-to-medium-range order in determining the properties of amorphous nanocatalysts is discussed. Current challenges faced in amorphous nanocatalysts are eventually summarized with several prospective research directions. By identifying the obstacles and potential avenues for further exploration, this perspective aims to contribute valuable insights that will propel the development of high-efficient amorphous nanocatalysts.</p></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"3 ","pages":"Article 100025"},"PeriodicalIF":0.0,"publicationDate":"2023-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49751049","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}
Shasha Guo , Chao Chen , Mengyi Qiu , Xun Cao , Zude Shi , Mingyu Ma , Jun Di , Shuzhou Li , Chao Zhu , Yongmin He , Zheng Liu
{"title":"Capping strategy for electrocatalysts with ultra-low platinum metal loading","authors":"Shasha Guo , Chao Chen , Mengyi Qiu , Xun Cao , Zude Shi , Mingyu Ma , Jun Di , Shuzhou Li , Chao Zhu , Yongmin He , Zheng Liu","doi":"10.1016/j.mtcata.2023.100022","DOIUrl":"https://doi.org/10.1016/j.mtcata.2023.100022","url":null,"abstract":"<div><p>The urgent demand for terawatt-scale clean energy necessitates the rational design of noble metal catalysts with minimal noble metal loading while maintaining high catalytic activity. However, the durability of low-loading catalysts is a critical concern for their successful industrial implementation. Here, we present a capping strategy using an amorphous HfO<sub>2</sub> (m-HfO<sub>2</sub>) to address this issue. Take Pt/C catalysts with Pt loading as low as 81.39 ng cm<sup>−2</sup> as an example, we demonstrate that the m-HfO<sub>2</sub> layer (10 nm) serves as an efficient mass transport channel for underneath Pt active sites, and effectively mitigates bubble-induced blockage of active sites by separating bubble formation sites with Pt active sites. Thus, the resulting catalyst exhibits a remarkable mass activity of 122.87 A mg<sup>−1</sup> and an overpotential of 11 mV at 10 mA cm<sup>−2</sup>. Furthermore, the m-HfO<sub>2</sub> plays a crucial role in eliminating the structural transformation and extending the lifetime of Pt-based catalysts, as evidenced by no loss of specific activity after consecutively cycling the catalyst for over 100 h. Such a capping strategy is potentially applied to other types of reactions and catalyst systems.</p></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"3 ","pages":"Article 100022"},"PeriodicalIF":0.0,"publicationDate":"2023-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49751048","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}
Hao Zhang , Tianyu Gao , Qizhao Zhang , Bang Gu , Qinghu Tang , Qiue Cao , Wenhao Fang
{"title":"Synergistic catalysis in loaded PtRu alloy nanoparticles to boost base-free aerobic oxidation of 5-hydroxymethylfurfural","authors":"Hao Zhang , Tianyu Gao , Qizhao Zhang , Bang Gu , Qinghu Tang , Qiue Cao , Wenhao Fang","doi":"10.1016/j.mtcata.2023.100013","DOIUrl":"https://doi.org/10.1016/j.mtcata.2023.100013","url":null,"abstract":"<div><p>The synergistic catalysis of dual metal sites is vital for selective activation of complicated chemical bonds in biomass compounds. The base-free selective oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) using air as oxidant and water as solvent is a highly sustainable upgrading process for cellulosic carbohydrates. In this work, a series of Pt<sub><em>x</em></sub>Ru-MgAlO (<em>x</em> = 0.5, 1, 2 and 3, in mole) nanocatalysts with controlled particle sizes (<em>ca.</em> 2 nm) were synthesized by a PVP-assisted adsorption method. The Pt<sub>2</sub>Ru-MgAlO catalyst showed 99% selectivity of FDCA with full conversion of HMF at only 100 °C under 0.2 MPa of air. In the meantime, an initial reaction rate of HMF of 2.8 mmol mol<sub>M</sub><sup>−1</sup> s<sup>−1</sup> and an intrinsic turnover frequency of 61.5 h<sup>−1</sup> were attained, respectively. Besides, this catalyst exhibited superior stability during five consecutive reuses without metal leaching. It was disclosed that the Pt-Ru interaction played critical roles in determining the intrinsic activity and the C<img>O bond activation of the prepared Pt<sub><em>x</em></sub>Ru-MgAlO catalysts. Kinetic experiments combined with <em>in situ</em> chemisorption techniques clearly unraveled adsorption and activation processes of C<img>O bond on Pt<sup>0</sup>-Ru<sup>0</sup> sites. To the best of our knowledge, this work firstly reported a PtRu bimetallic catalyst for aerobic oxidation of HMF and provided insight into synergistic catalysis.</p></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"3 ","pages":"Article 100013"},"PeriodicalIF":0.0,"publicationDate":"2023-08-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49765542","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}