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学者姓名:陈戈
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Abstract :
Hydrogen peroxide (H2O2) is a versatile and zero-emission material that is widely used in the industrial, domestic, and healthcare sectors. It is clear that it plays a critical role in advancing environmental sustainability, acting as a green energy source, and protecting human health. Conventional production techniques focused on anthraquinone oxidation, however, electrocatalytic synthesis has arisen as a means of utilizing renewable energy sources in conjunction with available resources like oxygen and water. These strides represent a substantial change toward more environmentally and energy-friendly H2O2 manufacturing techniques that are in line with current environmental and energy goals. This work reviews recent advances in two-electron water oxidation reaction (2e-WOR) electrocatalysts, including design principles and reaction mechanisms, examines catalyst design alternatives and experimental characterization techniques, proposes standardized assessment criteria, investigates the impact of the interfacial milieu on the reaction, and discusses the value of in situ characterization and molecular dynamics simulations as a supplement to traditional experimental techniques and theoretical simulations, as shown in Figure 1. The review also emphasizes the importance of device design, interface, and surface engineering in improving the production of H2O2. Through adjustments to the chemical microenvironment, catalysts can demonstrate improved performance, opening the door for commercial applications that are scalable through tandem cell development.
Keyword :
Interface Interface H2O2 H2O2 Electrolyte Electrolyte Electrocatalyst Electrocatalyst 2e-WOR 2e-WOR
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GB/T 7714 | Cao, Huixuan , Chen, Ge , Yan, Yong et al. Advances in Two-Electron Water Oxidation Reaction for Hydrogen Peroxide Production: Catalyst Design and Interface Engineering [J]. | CHEMSUSCHEM , 2024 . |
MLA | Cao, Huixuan et al. "Advances in Two-Electron Water Oxidation Reaction for Hydrogen Peroxide Production: Catalyst Design and Interface Engineering" . | CHEMSUSCHEM (2024) . |
APA | Cao, Huixuan , Chen, Ge , Yan, Yong , Wang, Dong . Advances in Two-Electron Water Oxidation Reaction for Hydrogen Peroxide Production: Catalyst Design and Interface Engineering . | CHEMSUSCHEM , 2024 . |
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Abstract :
负载型金属纳米粒子催化剂被广泛应用于化工工业生产中,但由于金属在高温环境中容易烧结而导致催化剂失活,因此提高催化剂的高温热稳定性是多相催化领域的重大挑战.本文概述了金属纳米颗粒的高温烧结机制:纳米粒子迁移-聚集过程(PMC)和Ostwald熟化(OR),讨论了近年来通过增强金属-载体相互作用、调节金属纳米粒子与包裹层之间的界面效应、构建多功能结构等方法在制备抗烧结型金属纳米催化剂方面的研究进展并对其进行总结.
Keyword :
高温热稳定性 高温热稳定性 烧结 烧结 催化剂工程 催化剂工程 金属纳米粒子 金属纳米粒子
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GB/T 7714 | 李淑贞 , 张桂臻 , 杨晓栋 et al. 抗烧结型金属纳米催化剂的制备策略 [J]. | 工业催化 , 2023 , 31 (7) : 1-14 . |
MLA | 李淑贞 et al. "抗烧结型金属纳米催化剂的制备策略" . | 工业催化 31 . 7 (2023) : 1-14 . |
APA | 李淑贞 , 张桂臻 , 杨晓栋 , 张龙 , 陈戈 , 邱文革 et al. 抗烧结型金属纳米催化剂的制备策略 . | 工业催化 , 2023 , 31 (7) , 1-14 . |
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Abstract :
New types of photocatalytic systems formed by coupling annealed large-sized NiFe-LDH nanosheets with smallsized TiO2 nanosheets were used to facilitate the rapid separation of photo-generated electrons and holes. The photocatalytic hydrogen production for optimized photocatalytic systems can reach 209 mmol/g, which is 8 times of that for TiO2. To understand the photocatalytic mechanism, in-situ annealing transmission electron microscopy (TEM) investigation of the microstructural evolution of large-sized NiFe-LDH nanosheets identified typical microstructures at different annealing stages. The microstructure of the optimized system contains plentiful ultrafine grains distributed along surface delaminated defects, which can provide abundant active sites for photocatalytic hydrogen evolution. Electrochemical and spectroscopic techniques were further used to determine the Z-scheme mechanism, guiding photo-generated electrons to fast transfer onto large-sized NiFeLDH nanosheets to achieve high efficient carrier separation.
Keyword :
TiO 2 nanosheet TiO 2 nanosheet In-situ TEM In-situ TEM Photocatalytic hydrogen Photocatalytic hydrogen NiFe nanosheet NiFe nanosheet Typical microstructure Typical microstructure
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GB/T 7714 | Gao, Chunlang , Li, Yuanli , Zhang, Zhenghan et al. Improving photocatalytic hydrogen production via ultrafine-grained precipitates formed nearby surface defects of NiFe-LDH nanosheets [J]. | CHEMICAL ENGINEERING JOURNAL , 2022 , 446 . |
MLA | Gao, Chunlang et al. "Improving photocatalytic hydrogen production via ultrafine-grained precipitates formed nearby surface defects of NiFe-LDH nanosheets" . | CHEMICAL ENGINEERING JOURNAL 446 (2022) . |
APA | Gao, Chunlang , Li, Yuanli , Zhang, Zhenghan , Li, Weiming , Zhong, Jiaxing , Zhang, Hang et al. Improving photocatalytic hydrogen production via ultrafine-grained precipitates formed nearby surface defects of NiFe-LDH nanosheets . | CHEMICAL ENGINEERING JOURNAL , 2022 , 446 . |
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The electrochemical production of hydrogen peroxide via the two-electron (2e(-)) oxygen reduction reaction (ORR) is an environmentally friendly method and is expected to be an alternative means to the industrial anthraquinone process. It is particularly suitable for on-site and small-scale H2O2 requirements. The development of earth-abundant catalysts with high activity and selectivity toward H2O2 is highly desirable and challenging. Here, we have prepared Co3O4 with tunable oxygen vacancies (OVs) and strongly coupled it to nitrogen-doped carbon nanotubes through an exsolution strategy. The Co3O4 with a higher OV concentration exhibits a higher 2e(-) ORR activity, higher H2O2 selectivity, and lower H2O2 reduction reaction (H2O2RR) activity so that effectively improving the production rate of H2O2 (1.6 mol peroxide/gcatalyst/h at 0.0 VRHE) in acidic media. The catalyst is also used as a cathode for the electro-Fenton process and degrades up to 80% of 40 mg/L of rhodamine B solution within 25 min. Density functional theory calculation shows that the *OOH binding energy (Delta G(*OOH)) could decrease on increasing the numbers of OVs, which subsequently benefits the protonation of *OOH to generate H2O2. (c) 2021 Elsevier Ltd. All rights reserved.
Keyword :
ORR ORR Cobaltosic oxide Cobaltosic oxide Hydrogen peroxide production Hydrogen peroxide production Oxygen vacancy Oxygen vacancy Exsolution Exsolution
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GB/T 7714 | Yan, Lina , Cheng, Xing , Wang, Yueshuai et al. Exsolved Co3O4 with tunable oxygen vacancies for electrocatalytic H2O2 production [J]. | MATERIALS TODAY ENERGY , 2022 , 24 . |
MLA | Yan, Lina et al. "Exsolved Co3O4 with tunable oxygen vacancies for electrocatalytic H2O2 production" . | MATERIALS TODAY ENERGY 24 (2022) . |
APA | Yan, Lina , Cheng, Xing , Wang, Yueshuai , Wang, Zhaozhao , Zheng, Lirong , Yan, Yong et al. Exsolved Co3O4 with tunable oxygen vacancies for electrocatalytic H2O2 production . | MATERIALS TODAY ENERGY , 2022 , 24 . |
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Innovatively designed, modified, and synthesized catalyst/electrode materials are of great importance in improving the performance of electrochemical energy devices for energy storage and conversion. Among various material modification technologies, the ion-irradiation technique has been recognized as a promising technology, which can effectively modify and design materials through controlling the key irradiation parameters, such as irradiation ion species, energy and fluence. The advantages of the ion-irradiation technique are high precision, favorable controllability, favorable repeatability, etc.; meanwhile, it can realize arbitrary element doping and defect control for many catalyst/electrode materials. Notably, it does not induce any impurities into the target materials during the ion-irradiation process, which is superior to many chemical modifications. The effects of ion-irradiation on catalyst/electrode materials in recent years are described in this review, including defect introduction, regulation of the electronic structure, morphology control, synthesis, and element doping. Then, the applications of ion irradiated catalyst/electrode materials in water electrolysis/photoelectrolysis cells, lithium-ion batteries, and supercapacitors are systematically summarized with an emphasis on the advantages of boosting the properties of materials. Finally, the challenges and strategies are proposed for developing more practical ion-irradiation techniques towards high-performance catalyst/electrode materials.
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GB/T 7714 | Wang, Yahui , Cheng, Xing , Zhang, Kai et al. Ion-irradiation of catalyst and electrode materials for water electrolysis/photoelectrolysis cells, rechargeable batteries, and supercapacitors [J]. | MATERIALS ADVANCES , 2022 , 3 (20) : 7384-7405 . |
MLA | Wang, Yahui et al. "Ion-irradiation of catalyst and electrode materials for water electrolysis/photoelectrolysis cells, rechargeable batteries, and supercapacitors" . | MATERIALS ADVANCES 3 . 20 (2022) : 7384-7405 . |
APA | Wang, Yahui , Cheng, Xing , Zhang, Kai , Chen, Ge , Wang, Ruzhi , Zhang, Jiujun . Ion-irradiation of catalyst and electrode materials for water electrolysis/photoelectrolysis cells, rechargeable batteries, and supercapacitors . | MATERIALS ADVANCES , 2022 , 3 (20) , 7384-7405 . |
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Abstract :
Developing oxide supports for stabilizing single-atom catalysts enables more flexibility for tuning the electronic metal-support interactions (EMSIs) toward better catalytic activities. However, due to the electronegativity of oxygen anions, single-metal atoms often remain positively charged in these oxide supports and are poor at binding hydrogen species for the hydrogen evolution reaction (HER). Here, we report a ligand charge donation-acquisition balance strategy via an amorphous TiBxOy support to tune the EMSIs, which lead to the boosted HER mass activity of a single Pt atom catalyst. Based on spectroscopic characterizations, we found that Pt single atoms preferentially bonded with nearly neutral B atoms originating from TiB2-like species in the Ti-B-O framework rather than O anions. Density functional theory calculations reveal that due to the charge-transfer balance between B-O and B-Pt, the nucleophilicity of Pt was tuned to an optimum state, with an ideal hydrogen binding energy that benefits the HER. As a result, this Pt/TiBxOy catalyst achieves a high HER mass activity (37.8 A mg(-1) Pt) and a turnover frequency (33.2 H-2 s(-1) Pt site(-1)) at an overpotential of 50 mV in an acid medium, outperforming commercial Pt/C by a factor of 34 and 33, respectively.
Keyword :
single atom single atom charge transfer charge transfer amorphous support amorphous support hydrogen evolution reaction hydrogen evolution reaction electronic metal-support interactions electronic metal-support interactions
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GB/T 7714 | Cheng, Xing , Xiao, Bo , Chen, Yanhui et al. Ligand Charge Donation-Acquisition Balance: A Unique Strategy to Boost Single Pt Atom Catalyst Mass Activity toward the Hydrogen Evolution Reaction [J]. | ACS CATALYSIS , 2022 , 12 (10) : 5970-5978 . |
MLA | Cheng, Xing et al. "Ligand Charge Donation-Acquisition Balance: A Unique Strategy to Boost Single Pt Atom Catalyst Mass Activity toward the Hydrogen Evolution Reaction" . | ACS CATALYSIS 12 . 10 (2022) : 5970-5978 . |
APA | Cheng, Xing , Xiao, Bo , Chen, Yanhui , Wang, Yueshuai , Zheng, Lirong , Lu, Yue et al. Ligand Charge Donation-Acquisition Balance: A Unique Strategy to Boost Single Pt Atom Catalyst Mass Activity toward the Hydrogen Evolution Reaction . | ACS CATALYSIS , 2022 , 12 (10) , 5970-5978 . |
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Nanosized Pd-based catalysts are widely used in the direct hydrogen peroxide (H2O2) synthesis from H-2 and O-2, while the selectivity and yield of H2O2 remain inferior. Here, a remarkable H2O2 yield of 115 mol/g(Pd)/h and H2O2 selectivity higher than 99% are reported using a Pd single-atom catalyst for the direct synthesis of H2O2. Nanosized palladium (Pd)-based catalysts are widely used in the direct hydrogen peroxide (H2O2) synthesis from H-2 and O-2, while its selectivity and yield remain inferior because of the O-O bond cleavage from both the reactant O-2 and the produced H2O2, which is assumed to have originated from various O-2 adsorption configurations on the Pd nanoparticles. Herein, single Pd atom catalyst with high activity and selectivity is reported. Density functional theory calculations certify that the O-O bond breaking is significantly inhibited on the single Pd atom and the O-2 is easier to be activated to form *OOH, which is a key intermediate for H2O2 synthesis; in addition, H2O2 degradation is shut down. Here, we show single Pd atom catalyst displays a remarkable H2O2 yield of 115 mol/g(Pd)/h and H2O2 selectivity higher than 99%; while the concentration of H2O2 reaches 1.07 wt.% in a batch.
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GB/T 7714 | Yu, Shiming , Cheng, Xing , Wang, Yueshuai et al. High activity and selectivity of single palladium atom for oxygen hydrogenation to H2O2 [J]. | NATURE COMMUNICATIONS , 2022 , 13 (1) . |
MLA | Yu, Shiming et al. "High activity and selectivity of single palladium atom for oxygen hydrogenation to H2O2" . | NATURE COMMUNICATIONS 13 . 1 (2022) . |
APA | Yu, Shiming , Cheng, Xing , Wang, Yueshuai , Xiao, Bo , Xing, Yiran , Ren, Jun et al. High activity and selectivity of single palladium atom for oxygen hydrogenation to H2O2 . | NATURE COMMUNICATIONS , 2022 , 13 (1) . |
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Reducing the usage of noble metals, such as platinum-based catalysts for oxygen reduction reaction (ORR) is pressingly demanded towards the practical applications of proton-exchange membrane fuel cells. One promising way is to develop Pt single atom catalysts (SACs), which, however, are plagued by their preference toward two-electron ORR pathway as well as stability issue. Herein, a single-atom alloy (SAA) catalyst with platinum-cobalt (Pt-Co) dual sites encapsulated in nitrogen-doped graphitized carbon nanotubes (Pt1Co100/N-GCNT) consisting of isolated Pt atoms decorated on the surface of Co nanoparticles was reported. Based on complementary spectroscopic characterizations and first-principle calculations, we propose that the unique Pt-Co dual sites in SAA facilitates the adsorption and dissociation of oxygen, particularly for the immobilization of OOH* intermediate and the dissociation of OH* intermediate, and thus result in high-efficiency four-electron ORR pathway. Consequently, the Pt1Co100/N-GCNT SAA catalyst achieves a mass activity of 0.81 A mg(Pt)(-1) at 0.90 V (versus the reversible hydrogen electrode) in 0.1 M HClO4 electrolyte, outperform commercial Pt/C catalyst for 5.4 times. The superior stability of the SAA catalyst was reflected by the results from the 30,000 potential-scanning cycles combined with the post characterization of the catalyst.
Keyword :
Single-atom alloy Single-atom alloy Pt-Co dual sites Pt-Co dual sites Operando XAS Operando XAS Oxygen reduction reaction Oxygen reduction reaction Electrocatalyst Electrocatalyst
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GB/T 7714 | Cheng, Xing , Wang, Yueshuai , Lu, Yue et al. Single-atom alloy with Pt-Co dual sites as an efficient electrocatalyst for oxygen reduction reaction [J]. | APPLIED CATALYSIS B-ENVIRONMENTAL , 2022 , 306 . |
MLA | Cheng, Xing et al. "Single-atom alloy with Pt-Co dual sites as an efficient electrocatalyst for oxygen reduction reaction" . | APPLIED CATALYSIS B-ENVIRONMENTAL 306 (2022) . |
APA | Cheng, Xing , Wang, Yueshuai , Lu, Yue , Zheng, Lirong , Sun, Shaorui , Li, Hongyi et al. Single-atom alloy with Pt-Co dual sites as an efficient electrocatalyst for oxygen reduction reaction . | APPLIED CATALYSIS B-ENVIRONMENTAL , 2022 , 306 . |
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Abstract :
Engineering the local coordination environment in atomically dispersed catalyst has proven to be a prospective route to boost catalyst performance for hydrogen evolution reaction (HER). Herein, we present the utilization of local lattice distortion of TiO2 support to regulate the local coordination environment and electronic structures of atomically dispersed Pt catalysts, resulting in the enhanced performance toward HER. Spectral analysis uncovers an elongated Pt–O bond length, lower Pt–O coordination numbers, as well as less electron holes residing in Pt 5d orbitals for Pt species on distorted TiO2. Density functional theory (DFT) calculation reveal that the variation might weaken the hydrogen adsorption on Pt sites and cause the optimized ΔG value of H∗. As a result, the atomically dispersed Pt catalyst displays superior HER mass activity (62.34 A mg−1 Pt) and the highest turnover frequency (TOF) (56.1H2·s−1) at the 50 mV overpotential in an acid media that are 18.7 and 5.56 times higher than commercial Pt/C. The work should create a new avenue in manipulating the local coordination environment of catalysts via the lattice distortion of the support, and in pursuing desired catalytic performance. © 2021 Elsevier Ltd
Keyword :
Coordination reactions Coordination reactions Catalyst supports Catalyst supports Electronic structure Electronic structure Density functional theory Density functional theory Bond length Bond length Hydrogen evolution reaction Hydrogen evolution reaction Platinum Platinum Gas adsorption Gas adsorption Spectrum analysis Spectrum analysis Oxide minerals Oxide minerals Hydrogen Hydrogen Titanium dioxide Titanium dioxide
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GB/T 7714 | Cheng, Xing , Lu, Yue , Zheng, Lirong et al. Engineering local coordination environment of atomically dispersed platinum catalyst via lattice distortion of support for efficient hydrogen evolution reaction [J]. | Materials Today Energy , 2021 , 20 . |
MLA | Cheng, Xing et al. "Engineering local coordination environment of atomically dispersed platinum catalyst via lattice distortion of support for efficient hydrogen evolution reaction" . | Materials Today Energy 20 (2021) . |
APA | Cheng, Xing , Lu, Yue , Zheng, Lirong , Pupucevski, Max , Li, Hongyi , Chen, Ge et al. Engineering local coordination environment of atomically dispersed platinum catalyst via lattice distortion of support for efficient hydrogen evolution reaction . | Materials Today Energy , 2021 , 20 . |
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In this study, we employed in situ liquid cell transmission electron microscopy (LC-TEM) to carry out a new design strategy of precisely regulating the microstructure of large-sized cocatalysts for highly efficient energy harvesting. This unique strategy was conducted by dynamically in situ monitoring the entire process of the galvanic replacement reaction between Cu nanowires and Au ion solutions to reveal the detailed microstructural evolution at the nanometer scale, which has never been achieved by conventional chemical methods. Based on the strategy, four kinds of cocatalysts were designed and fabricated, which have typical structural characteristics that correspond to different reaction stages. By coupling them with ultrafine photocatalysts to construct photocatalytic systems, the photocatalytic hydrogen production of the optimized system is 65 times higher than that of the counterpart photocatalysts, strongly demonstrating the feasibility of the design via in situ liquid cell TEM. The strategy here provides an innovative way to design new kinds of catalytic systems.
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GB/T 7714 | Gao, Chunlang , Zhuang, Chunqiang , Li, Yuanli et al. In situ liquid cell transmission electron microscopy guiding the design of large-sized cocatalysts coupled with ultra-small photocatalysts for highly efficient energy harvesting [J]. | JOURNAL OF MATERIALS CHEMISTRY A , 2021 , 9 (22) : 13056-13064 . |
MLA | Gao, Chunlang et al. "In situ liquid cell transmission electron microscopy guiding the design of large-sized cocatalysts coupled with ultra-small photocatalysts for highly efficient energy harvesting" . | JOURNAL OF MATERIALS CHEMISTRY A 9 . 22 (2021) : 13056-13064 . |
APA | Gao, Chunlang , Zhuang, Chunqiang , Li, Yuanli , Qi, Heyang , Chen, Ge , Sun, Zaicheng et al. In situ liquid cell transmission electron microscopy guiding the design of large-sized cocatalysts coupled with ultra-small photocatalysts for highly efficient energy harvesting . | JOURNAL OF MATERIALS CHEMISTRY A , 2021 , 9 (22) , 13056-13064 . |
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