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Advances in Two-Electron Water Oxidation Reaction for Hydrogen Peroxide Production: Catalyst Design and Interface Engineering SCIE
期刊论文 | 2024 , 18 (2) | CHEMSUSCHEM
WoS CC Cited Count: 1
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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 , 18 (2) .
MLA Cao, Huixuan et al. "Advances in Two-Electron Water Oxidation Reaction for Hydrogen Peroxide Production: Catalyst Design and Interface Engineering" . | CHEMSUSCHEM 18 . 2 (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 , 18 (2) .
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抗烧结型金属纳米催化剂的制备策略
期刊论文 | 2023 , 31 (7) , 1-14 | 工业催化
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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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一种用于电解水氧化合成过氧化氢的碳基催化剂的制备方法 incoPat zhihuiya
专利 | 2023-02-20 | CN202310138624.9
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Abstract :

一种用于电解水氧化合成过氧化氢的碳基催化剂的制备方法涉及电催化领域,解决现有催化剂过电位高,选择性低,产率不足,产量无法达到工业生产水平的问题。本发明采用的是高温煅烧法,通过控制材料煅烧条件,仅改变所添加聚四氟乙烯与三聚氰胺的用量比,就能得到具有3D结构形貌的高产率低过电位的碳基催化材料,更大的相对表面积及空间个异性使得电子快速传输和逸出。元素F掺杂降低了电荷转移势垒,加速了电子‑空穴的分离和迁移,量子效率显著增加,同时改变了三相界面疏水性能,有效抑制副反应,选择性得以提升。

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GB/T 7714 陈戈 , 曹会选 . 一种用于电解水氧化合成过氧化氢的碳基催化剂的制备方法 : CN202310138624.9[P]. | 2023-02-20 .
MLA 陈戈 et al. "一种用于电解水氧化合成过氧化氢的碳基催化剂的制备方法" : CN202310138624.9. | 2023-02-20 .
APA 陈戈 , 曹会选 . 一种用于电解水氧化合成过氧化氢的碳基催化剂的制备方法 : CN202310138624.9. | 2023-02-20 .
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一种基于分子尺度设计的原子层沉积法制备碳基电催化剂的方法 incoPat zhihuiya
专利 | 2023-02-20 | CN202310138623.4
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Abstract :

一种基于分子尺度设计的原子层沉积法制备碳基电催化剂的方法涉及电催化领域,解决现有合成方法步骤繁杂,控制条件多,材料不稳定,导电性能较差及产率较低等问题。本发明采用高温煅烧法制备疏水碳材料基底,采用原子层沉积法对材料进行进一步的表面改性,仅改变所沉积前驱体Ti的沉积圈数即可制备出一系列催化剂。通过F、Ti双掺杂对分子层面活性位点的调控,影响三相界面反应路径,降低电荷转移的势垒,量子效率显著增加,同时,结构致密且厚度可控的沉积层在保证催化剂电解性能的同时,对材料循环稳定性也有很大提升。出于对工业化应用中的实际需求考虑,本发明是一种原料低廉易得且结构稳定的适用于生产实践的碳基催化剂制备方法。

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GB/T 7714 陈戈 , 曹会选 . 一种基于分子尺度设计的原子层沉积法制备碳基电催化剂的方法 : CN202310138623.4[P]. | 2023-02-20 .
MLA 陈戈 et al. "一种基于分子尺度设计的原子层沉积法制备碳基电催化剂的方法" : CN202310138623.4. | 2023-02-20 .
APA 陈戈 , 曹会选 . 一种基于分子尺度设计的原子层沉积法制备碳基电催化剂的方法 : CN202310138623.4. | 2023-02-20 .
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High activity and selectivity of single palladium atom for oxygen hydrogenation to H2O2 SCIE
期刊论文 | 2022 , 13 (1) | NATURE COMMUNICATIONS
WoS CC Cited Count: 78
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Abstract :

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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Ligand Charge Donation-Acquisition Balance: A Unique Strategy to Boost Single Pt Atom Catalyst Mass Activity toward the Hydrogen Evolution Reaction SCIE
期刊论文 | 2022 , 12 (10) , 5970-5978 | ACS CATALYSIS
WoS CC Cited Count: 32
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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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Exsolved Co3O4 with tunable oxygen vacancies for electrocatalytic H2O2 production SCIE
期刊论文 | 2022 , 24 | MATERIALS TODAY ENERGY
WoS CC Cited Count: 39
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Abstract :

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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Ion-irradiation of catalyst and electrode materials for water electrolysis/photoelectrolysis cells, rechargeable batteries, and supercapacitors
期刊论文 | 2022 , 3 (20) , 7384-7405 | MATERIALS ADVANCES
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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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Improving photocatalytic hydrogen production via ultrafine-grained precipitates formed nearby surface defects of NiFe-LDH nanosheets SCIE
期刊论文 | 2022 , 446 | CHEMICAL ENGINEERING JOURNAL
WoS CC Cited Count: 30
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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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Single-atom alloy with Pt-Co dual sites as an efficient electrocatalyst for oxygen reduction reaction SCIE
期刊论文 | 2022 , 306 | APPLIED CATALYSIS B-ENVIRONMENTAL
WoS CC Cited Count: 124
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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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