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学者姓名：陈戈
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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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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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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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Abstract ：
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 ：
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 ：
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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Abstract ：
The urea-assisted water electrolysis reactions are of great significance for solving the increasingly serious energy crisis and environmental pollution. Recently, the photo-driven effect strategy has been demonstrated to be an efficient external driving force for improving electrocatalytic activities. Herein, we synthesized Ni-NiO heterostructured nanosheet arrays grown on Ni foam (denoted as Ni-NiO/NF) as a bifunctional electrocatalyst enhancing the urea oxidation reaction (UOR) and hydrogen evolution reaction (HER) activities simultaneously under light irradiation. Moreover, when the catalyst is used in a two-electrode system for the urea-assisted water electrolysis reaction, the cell potential could be reduced to 1.48 V to achieve the current density of 10 mA cm(-2) after exposure to light irradiation, as well as remarkable stability. Our studies demonstrate that the enhancement of the HER & UOR activities is attributed to a synergetic effect between photogenerated carriers and photothermy.
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| GB/T 7714 | Wang, Qi , Cheng, Xing , Sun, Yukun et al. A synergetic effect between photogenerated carriers and photothermally enhanced electrochemical urea-assisted hydrogen generation on the Ni-NiO/Nickel Foam catalyst [J]. | MATERIALS ADVANCES , 2021 , 2 (6) : 2104-2111 . |
| MLA | Wang, Qi et al. "A synergetic effect between photogenerated carriers and photothermally enhanced electrochemical urea-assisted hydrogen generation on the Ni-NiO/Nickel Foam catalyst" . | MATERIALS ADVANCES 2 . 6 (2021) : 2104-2111 . |
| APA | Wang, Qi , Cheng, Xing , Sun, Yukun , Sun, Zaicheng , Wang, Dong , Chen, Ge et al. A synergetic effect between photogenerated carriers and photothermally enhanced electrochemical urea-assisted hydrogen generation on the Ni-NiO/Nickel Foam catalyst . | MATERIALS ADVANCES , 2021 , 2 (6) , 2104-2111 . |
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Abstract ：
Solar water evaporation is a sustainable and efficient way to produce fresh water. Identifying highly efficient photothermal materials is an important step for achieving high evaporation rates. However, the effects of the water interfacial area are rarely paid any attention, although a few reports have demonstrated high evaporation rates from micro-/nanostructured devices. In this work, we introduce a new term, water mass per unit surface area (WMUA), to connect the water mass and interfacial area. We can regulate WMUA using different commercial porous materials to realize water management in devices, which further affects the evaporation rates. The optimized device is composed of suedette sponge, filter paper, and polydopamine as the water-transportation, water-restrictive, and photothermal materials, respectively, and it achieves an evaporation rate of 1.8 kg m−2h−1and energy efficiency of ∼92%. This presents a new strategy for the rational design of device structures and the promotion of evaporation rates, pushing this field into new areas. © The Royal Society of Chemistry 2021.
Keyword ：
Materials handling Materials handling Porous materials Porous materials Water management Water management Oceanography Oceanography Energy efficiency Energy efficiency Evaporation Evaporation
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| GB/T 7714 | Sun, Yukun , Zong, Xupeng , Qu, Dan et al. Water management by hierarchical structures for highly efficient solar water evaporation [J]. | Journal of Materials Chemistry A , 2021 , 9 (11) : 7122-7128 . |
| MLA | Sun, Yukun et al. "Water management by hierarchical structures for highly efficient solar water evaporation" . | Journal of Materials Chemistry A 9 . 11 (2021) : 7122-7128 . |
| APA | Sun, Yukun , Zong, Xupeng , Qu, Dan , Chen, Ge , An, Li , Wang, Xiayan et al. Water management by hierarchical structures for highly efficient solar water evaporation . | Journal of Materials Chemistry A , 2021 , 9 (11) , 7122-7128 . |
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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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Abstract ：
The development of economical, highly active, and robust electrocatalysts for oxygen evolution reaction (OER) is one of the major obstacles for producing affordable water splitting systems and metal-air batteries. Herein, it is reported that the subnanometric CoOx clusters with high oxidation state substitutionally dispersed in the lattice of rutile TiO2 support (Co-TiO2) can be prepared by a thermally induced phase segregation process. Owing to the strong interaction of CoOx clusters and TiO2 support, Co-TiO2 exhibits both excellent intrinsic activity and durability for OER. The turnover frequency of Co-TiO2 is up to 3.250 s−1 at overpotentials of 350 mV; this value is one of the highest in terms of OER performance among the current Co-based active materials under similar testing conditions; moreover, the OER current density loss is only 6.5% at a constant overpotential of 400 mV for 30 000 s, which is superior to the benchmark Co3O4 and RuO2 catalysts. Mechanism analysis demonstrates that charge transfer occurs between Co sites and their neighboring Ti atoms, triggering the efficient Co-Ti cooperative catalytic centers, in which OH* and O* are preferred to be adsorbed on the bridging sites of Co and Ti with favorable adsorption energy, inducing a lower energy barrier for O2 generation. © 2020 Wiley-VCH GmbH
Keyword ：
Electrocatalysts Electrocatalysts Binary alloys Binary alloys Benchmarking Benchmarking Catalytic oxidation Catalytic oxidation Oxide minerals Oxide minerals Ruthenium compounds Ruthenium compounds Cobalt Cobalt Metal-air batteries Metal-air batteries Oxygen Oxygen Titanium Titanium Titanium dioxide Titanium dioxide Charge transfer Charge transfer Oxygen evolution reaction Oxygen evolution reaction
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| GB/T 7714 | Yan, Yong , Liu, Chunyue , Jian, Hanwen et al. Substitutionally Dispersed High-Oxidation CoOx Clusters in the Lattice of Rutile TiO2 Triggering Efficient Co-Ti Cooperative Catalytic Centers for Oxygen Evolution Reactions [J]. | Advanced Functional Materials , 2021 , 31 (9) . |
| MLA | Yan, Yong et al. "Substitutionally Dispersed High-Oxidation CoOx Clusters in the Lattice of Rutile TiO2 Triggering Efficient Co-Ti Cooperative Catalytic Centers for Oxygen Evolution Reactions" . | Advanced Functional Materials 31 . 9 (2021) . |
| APA | Yan, Yong , Liu, Chunyue , Jian, Hanwen , Cheng, Xing , Hu, Ting , Wang, Dong et al. Substitutionally Dispersed High-Oxidation CoOx Clusters in the Lattice of Rutile TiO2 Triggering Efficient Co-Ti Cooperative Catalytic Centers for Oxygen Evolution Reactions . | Advanced Functional Materials , 2021 , 31 (9) . |
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