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Synthesis and In-Depth Characterization of Supported and Highly Dispersed Catalysts

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A special issue of Catalysts (ISSN 2073-4344). This special issue belongs to the section "Catalytic Materials".

Deadline for manuscript submissions: closed (31 December 2023) | Viewed by 20632

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Special Issue Editors

Dr. Zhongzhe Wei

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Guest Editor

Institute of Industrial Catalysis, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou 310032, China
Interests: heterogeneous catalysis; selective hydrogenation; catalysts design

Dr. Yutong Gong

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Guest Editor

State Key Laboratory of Solidification Processing, Northwestern Polytechnical University, Xi’an 710072, China
Interests: nanomaterials; materials genome; electrocatalysis; hetrogeneous catalysis; energy storage
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Special Issue Information

Dear Colleagues,

Catalysts, especially metallic catalysts, constitute one of the most important components in the conversion of chemical raw materials and play a dominant role in industrial applications for the production of highly valuable chemicals. The development of new materials holds the key to fundamental advancements in catalysis, both of which are vital in order to meet the challenge of environmental and energy crises. The dispersion of metal is an important issue in the design of heterogeneous catalysts. Highly dispersed catalysts can realize the full exposure and maximum utilization of active sites. To obtain highly dispersed catalysts, many strategies have been developed, such as the modification of supports, the grafting of organic molecules on metal surfaces, the partial coverage of active metal surfaces by metal oxides, the confinement of active metal nanoparticles in the micro- or mesopores of supports, the formation of bimetallic alloys or intermetallics or core–shell structures, and the construction of single-atom catalysts. Recently, with the development of certain spectroscopic measurements, for example, in situ Raman and X-ray absorption spectra, the structure evolution of catalysts during a reaction and real catalytic active sites have been explored. This Special Issue is devoted to the synthesis and in-depth characterization of supported and highly dispersed catalysts, issues associated with new strategies in the synthesis of supported and highly dispersed catalysts, and in situ characterization during reactions. We welcome reviews and original research papers regarding topics from fundamental to industrial applications on supported and highly dispersed catalysts with potential application in useful transformations. The potential topics include but are not limited to:

Methods for the synthesis and characterization of heterogeneous catalysts;
In situ spectroscopic measurement equipment applied in catalysis;
The evolution of supported active sites in catalysis with various in situ spectroscopic techniques;
Recent developments in advanced nanocatalysts;
Name reactions catalyzed by nanocatalysts;
Diverse catalytic transformations catalyzed by nanocatalysts;
Supported and highly dispersed catalysts for electrocatalytic reactions, such as HER, OER, etc.;
Supported and highly dispersed catalysts for photocatalytic reactions, such as HER, OER, etc.;
Oxidation and reduction reactions by nanocatalysts;
Cross-coupling and tandem reactions by nanocatalysts.

Dr. Zhongzhe Wei
Dr. Yutong Gong
Guest Editors

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Keywords

supported catalysts
highly dispersed catalysts
heterogeneous catalytic reactions
characterization of catalysts
structure evolution of catalysts in catalysis
in situ spectroscopic techniques

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Published Papers (10 papers)

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Research

17 pages, 4103 KiB

Open AccessEditor’s ChoiceArticle

Facile Synthesis of Silicon-Based Materials Modified Using Zinc(Ⅱ) 2-Bromoacetic as Heterogeneous Catalyst for the Fixation of CO₂ into Cyclic Carbonates

by Chaokun Yang, Xiangning Ma, Meng Li, Tuantuan Yang and Xin Zhao

Catalysts 2023, 13(7), 1116; https://doi.org/10.3390/catal13071116 - 17 Jul 2023

Cited by 3 | Viewed by 1443

Abstract

Much effort has been devoted to the development of efficient heterogeneous catalysts for the conversion of carbon dioxide (CO₂) into high-value chemicals. Generally, the cycloaddition of CO₂ to epoxides is considered a green and atom-economic reaction for the production of cyclic carbonates. Based on this, three kinds of silicon-based catalysts modified using zinc(Ⅱ) 2-bromoacetic (Si-ZnBA-n, n = 1, 2, 3) were facilely synthesized and employed for the chemical fixation of CO₂ to epoxides with the use of potassium iodide (KI). A series of characterization techniques were used to characterize the textual structures and physicochemical properties of Si-ZnBA-n. The synergistic effects of Zn, –NH_2, –OH and the nucleophilic group guaranteed the catalytic activity of Si-ZnBA-n. Si-ZnBA-1 exhibited the best catalytic activity among Si-ZnBA-n because Si-ZnBA-1 possessed the highest Zn content. Additionally, the effects of the reaction conditions (temperature, pressure, time and catalyst loadings) were also discussed. The propylene carbonate (PC) yield could reach 97% under 130 °C, 2 MPa, for 5 h without the employment of organic solvent, and its selectivity was 99%. In addition, the recycling property of Si-ZnBA-1/KI was also investigated, and the catalytic system exhibited good cycle performance. Meanwhile, the catalyst showed outstanding versatility for CO₂ application to various epoxides, and a possibly synergistic reaction mechanism was proposed. Finally, a dynamic model was developed to discuss the activation energy of the CO₂ cycloaddition reaction over the Si-ZnBA-1 catalyst. Full article

(This article belongs to the Special Issue Synthesis and In-Depth Characterization of Supported and Highly Dispersed Catalysts)

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10 pages, 3308 KiB

Open AccessCommunication

Au Nanoparticles Supported on Mn- or/and La-Doped CeO₂ Nanorods for One-Step Oxidative Esterification of Methacrolein and Methanol to Methyl Methacrylate

by Haojian Zhang

Catalysts 2023, 13(4), 767; https://doi.org/10.3390/catal13040767 - 18 Apr 2023

Cited by 1 | Viewed by 1541

Abstract

Mn- or/and La-doped CeO₂ nanorods supporting Au catalysts were prepared using the hydrothermal method and deposition precipitation (DP) method and applied to the direct oxidative esterification of methacrolein (MAL) and methanol into methyl methacrylate (MMA). Various characterization techniques such as N₂-physical adsorption, X-ray diffraction (XRD), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), H₂ temperature programmed reduction (TPR) and CO₂ temperature programmed desorption (TPD) were utilized to analyze the structural properties, reducibility and basicity of Au catalysts. The catalyst with Mn doping only showed the best performance, and particularly the highest conversion, while the catalyst with Mn and La doping showed the highest selectivity. Full article

(This article belongs to the Special Issue Synthesis and In-Depth Characterization of Supported and Highly Dispersed Catalysts)

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13 pages, 3790 KiB

Open AccessFeature PaperArticle

Petal-like g-C₃N₄ Enhances the Photocatalyst Removal of Hexavalent Chromium

by Huijuan Yu, Qiang Ma, Cuiping Gao, Shaohua Liao, Yingjie Zhang, Hong Quan and Ruiqi Zhai

Catalysts 2023, 13(3), 641; https://doi.org/10.3390/catal13030641 - 22 Mar 2023

Cited by 7 | Viewed by 2228

Abstract

The rapid progress of modern industry not only brings convenience to people’s lives, but also brings negative effects. Industrial development produces a large amount of waste metal, which brings harm to the environment and human health. Carbon nitride (g-C₃N₄) was successfully prepared using the thermal-polymerization method and petal-like g-C₃N₄ (CA-g-C₃N₄) was impregnated with citric acid (CA). Compared with g-C₃N₄, CA-g-C₃N₄ showed extremely high photocatalytic activity because the petal-like g-C₃N₄ (CA-g-C₃N₄) had a larger specific surface area, which increased the active sites on the surface of the photocatalyst and improved the photocatalytic activity. After citric acid treatment, the removal of hexavalent chromium (Cr(VI)) by g-C₃N₄ increased from 48% to 93%. The photocatalytic materials were characterized using X-ray diffraction (XRD), scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), Brunauer–Emmett–Teller (BET) and UV-vis diffuse reflectance spectra (UV-vis). In summary, this study confirmed that citric acid can improve the photocatalytic activity of g-C₃N₄ by increasing its specific surface area and the active site of the photocatalytic material so as to achieve the purpose of removing hexavalent chromium from water. Full article

(This article belongs to the Special Issue Synthesis and In-Depth Characterization of Supported and Highly Dispersed Catalysts)

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13 pages, 3624 KiB

Open AccessArticle

The Promotional Effect of Na on Ru for pH-Universal Hydrogen Evolution Reactions

by Bingxin Guo, Chengfei Zhao, Yingshuang Zhou, Junjie Guo, Zhongzhe Wei and Jing Wang

Catalysts 2023, 13(3), 552; https://doi.org/10.3390/catal13030552 - 9 Mar 2023

Cited by 1 | Viewed by 2366

Abstract

Alkali metals, as ideal electron donors, can effectively regulate the valence state distribution of the host metals. Nevertheless, no studies have reported the application of alkali metal promoters in the hydrogen evolution reaction (HER). Here, we designed an efficient and wide pH-universal hydrogen evolution catalyst that utilizes alkali metal to control the valence, size, and dispersion of Ru NPs. The experimental results reveal that the alkali metal additives contribute to the dispersion and stabilization of metallic Ru. More importantly, the interaction between Na and Ru regulates the distribution of Ru valence states and helps to form more active components of Ru⁰. Additionally, NaCl functioned as an in situ template to assist the construction of a porous carbon skeleton promotes mass transfer and exposes more active sites, further promoting the synergistic effect of Ru and Na. As a result, the optimal Ru_0.3/C−800 delivers high efficiency for HER with an overpotential as low as 29 mV in 1.0 M KOH and 83 mV in 0.5 M H₂SO₄ under 10 mA cm⁻². Particularly, the catalytic performance of Ru_0.3/C−800 even outbalanced that of commercial Pt/C in an alkaline medium. This rational construction strategy opens up new avenues for obtaining superior pH-universal electrocatalysts. Full article

(This article belongs to the Special Issue Synthesis and In-Depth Characterization of Supported and Highly Dispersed Catalysts)

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13 pages, 4859 KiB

Open AccessArticle

Unraveling the Mechanism for H₂O₂ Photogeneration on Polymeric Carbon Nitride with Alkali Metal Modification

by Zehao Li and Yufei Chen

Catalysts 2023, 13(2), 218; https://doi.org/10.3390/catal13020218 - 17 Jan 2023

Cited by 2 | Viewed by 1524

Abstract

K and Na have been widely used in photocatalytic H₂O₂ production. However, Rb and Cs have rarely been studied for their photocatalytic potentials. In addition, the mechanism regulating H₂O₂ production from different alkali metal (M)-modified polymeric carbon nitride (PCN) is still unknown. Therefore, M-doped PCN was fabricated using thermal copolymerization in the presence of Li, Na, K, Rb, or Cs. The activity of CN-M was enhanced by the increase in the metallic character of alkali metals. However, CN-Cs’s photocatalytic H₂O₂ activity is not optimal even though it has the strongest metallic character. A stronger metallic character is anticipated to yield stronger Lewis acidic sites. Although ethanol can be adsorbed and activated at strong Lewis acidic sites, H₂O₂ can also be activated at these sites, which speeds up H₂O₂ degradation. CN-Rb—with its acceptable metallic character, excellent oxygen adsorption capacity, and reduced H₂O₂ degradation—has the best photocatalytic H₂O₂ yield. Full article

(This article belongs to the Special Issue Synthesis and In-Depth Characterization of Supported and Highly Dispersed Catalysts)

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12 pages, 5630 KiB

Open AccessArticle

Protein-Carbonized Engineering to Construct Three-Dimensional Sponge-like Carbons for Oxygen Reduction Electrocatalysis

by Xinyi Luo, Yao Liu, Wenli Liao, Zhongbin Li, Chaozhong Guo, Wei Sun and Zhongli Luo

Catalysts 2023, 13(1), 166; https://doi.org/10.3390/catal13010166 - 10 Jan 2023

Viewed by 1740

Abstract

The low specific surface area and insufficient exposure of active sites are usually the key reasons for the poor oxygen reduction reaction of catalysts. Here, we update a new method, using NaCl as a template, egg white as a carbon source and nitrogen source, adding FeCl₃ as an iron source, and adopting a two-step pyrolysis method to synthesize a sponge-like porous Fe-N-C catalyst. This kind of three-dimensional sponge-like catalyst exhibits more defective structures, so it shows an excellent electrochemical performance with a half-wave potential of 0.73 V and onset potential of 0.88 V. Additionally, the catalyst has amazing stability, which proves that it is a promising candidate for green energy devices. Our research provides an innovative method to synthesize high-performance Fe-N-C catalysts using low-cost common biomaterials. Full article

(This article belongs to the Special Issue Synthesis and In-Depth Characterization of Supported and Highly Dispersed Catalysts)

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13 pages, 3783 KiB

Open AccessArticle

Exploring Deep Learning for Metalloporphyrins: Databases, Molecular Representations, and Model Architectures

by An Su, Chengwei Zhang, Yuan-Bin She and Yun-Fang Yang

Catalysts 2022, 12(11), 1485; https://doi.org/10.3390/catal12111485 - 21 Nov 2022

Cited by 4 | Viewed by 2281

Abstract

Metalloporphyrins have been studied as biomimetic catalysts for more than 120 years and have accumulated a large amount of data, which provides a solid foundation for deep learning to discover chemical trends and structure–function relationships. In this study, key components of deep learning of metalloporphyrins, including databases, molecular representations, and model architectures, were systematically investigated. A protocol to construct canonical SMILES for metalloporphyrins was proposed, which was then used to represent the two-dimensional structures of over 10,000 metalloporphyrins in an existing computational database. Subsequently, several state-of-the-art chemical deep learning models, including graph neural network-based models and natural language processing-based models, were employed to predict the energy gaps of metalloporphyrins. Two models showed satisfactory predictive performance (R² 0.94) with canonical SMILES as the only source of structural information. In addition, an unsupervised visualization algorithm was used to interpret the molecular features learned by the deep learning models. Full article

(This article belongs to the Special Issue Synthesis and In-Depth Characterization of Supported and Highly Dispersed Catalysts)

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14 pages, 3044 KiB

Open AccessArticle

Computational Insight into Defective Boron Nitride Supported Double-Atom Catalysts for Electrochemical Nitrogen Reduction

by Rong Cao, Jie-Zhen Xia and Qi Wu

Catalysts 2022, 12(11), 1404; https://doi.org/10.3390/catal12111404 - 10 Nov 2022

Cited by 4 | Viewed by 2185

Abstract

Designing highly selective and efficient double-atom electrocatalysts (DACs) is essential for achieving a superior nitrogen-reduction reaction (NRR) performance. Herein, we explored the defective boron nitride–supported cage-like double-atom catalysts to rummage the qualified NRR catalysts. Based on a systematic evaluation of the stability, N₂ adsorption, NRR selectivity and activity of 10 DACs of TM₁-TM₂@V_B-BN, we predicted Ru-Ti@V_B-BN to be the NRR candidate with a limiting potential of −0.40 V. Compared to the corresponding single-atom catalysts, the introduction of Ti/Mo modulates the d-band center of the active metal atom, which improves the NRR performance. Moreover, the magnetic Ru-Ti dimer can facilitate the transfer of charge to molecular N₂, ensuring a significant activation of the inert N≡N bond. This research not only opens up new avenues for designing boron nitride–supported DACs for NRR, but also deepens the understanding of DACs in N₂ activation. Full article

(This article belongs to the Special Issue Synthesis and In-Depth Characterization of Supported and Highly Dispersed Catalysts)

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19 pages, 8368 KiB

Open AccessArticle

Core-Shell Hierarchical Fe/Cu Bimetallic Fenton Catalyst with Improved Adsorption and Catalytic Performance for Congo Red Degradation

by Haimei Chen, Shaofei Wang, Lilan Huang, Leitao Zhang, Jin Han, Wanzheng Ren, Jian Pan and Jiao Li

Catalysts 2022, 12(11), 1363; https://doi.org/10.3390/catal12111363 - 4 Nov 2022

Cited by 7 | Viewed by 1839

Abstract

The preparation of heterogeneous Fenton catalysts with both adsorption and catalytic properties has become an effective strategy for the treatment of refractory organic wastewater. In this work, 4A-Fe@Cu bimetallic Fenton catalysts with a three-dimensional core-shell structure were prepared by a simple, template-free, and surfactant-free methodology and used in the adsorption and degradation of Congo red (CR). The results showed that the open three-dimensional network structure and the positive charge of the surface of the 4A-Fe@Cu catalyst could endow a high adsorption capacity for CR, reaching 432.9 mg/g. The good adsorption property of 4A-Fe@Cu for CR not only did not inactivate the catalytic site on 4A-Fe@Cu but also could promote the contact between CR and the active sites on the catalyst surface and accelerate the degradation process. The 4A-Fe@Cu bimetallic catalyst exhibited higher catalytic activity than monometallic 4A@Cu and/or 4A-Fe catalysts due to low work function value. The effects of different pH, H₂O₂ dosages, and catalyst dosages on the catalytic performance of 4A-Fe@Cu were explored. In the conditions of 7.2 mM H₂O₂, 2 g/L 4A-Fe@Cu, and 1 g/L CR solution, the degradation ratio of CR by 4A-Fe@Cu could reach 99.2% at pH 8. This strategy provided guidance to the design of high-performance Fenton-like catalysts with both adsorption and catalysis properties for dye wastewater treatment. Full article

(This article belongs to the Special Issue Synthesis and In-Depth Characterization of Supported and Highly Dispersed Catalysts)

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13 pages, 6040 KiB

Open AccessArticle

Boron and Phosphorus Co-Doped Graphitic Carbon Nitride Cooperate with Bu₄NBr as Binary Heterogeneous Catalysts for the Cycloaddition of CO₂ to Epoxides

by Chaokun Yang, Xin Zhao and Tuantuan Yang

Catalysts 2022, 12(10), 1196; https://doi.org/10.3390/catal12101196 - 8 Oct 2022

Cited by 4 | Viewed by 2361

Abstract

The development of a cost-effective heterogeneous catalytic system for the cycloaddition reaction of CO₂ and epoxides is of great importance. In this manuscript, three kinds of boron and phosphorus co-doping graphitic carbon nitride (BP-CN) were prepared and characterized. Among them, BP-CN-1 displayed the optimal catalytic performance in the presence of Bu₄NBr (tetrabutylammonium bromide) for the CO₂ cycloaddition with propylene oxide, and 95% propylene carbonate yield was obtained under a 120 °C, 2 MPa, 6 h condition. Moreover, the BP-CN-1/Bu₄NBr catalytic system is compatible with various epoxides and also exhibits excellent recycling performance under metal- and solvent-free conditions. Hence, BP-CN-1 exhibited an attractive application for the efficient fixation of CO₂ due to the simple, eco-friendly synthesis route and effective catalytic activity. Full article

(This article belongs to the Special Issue Synthesis and In-Depth Characterization of Supported and Highly Dispersed Catalysts)

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