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学者姓名：王凯文
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Abstract ：
Hydrogen storage has long been a priority on the renewable energy research agenda. Due to its high volumetric and gravimetric hydrogen density, MgH2 is a desirable candidate for solid-state hydrogen storage. However, its practical use is constrained by high thermal stability and sluggish kinetics. Here, PdNi bilayer metallenes are reported as catalysts for hydrogen storage of bulk-MgH2 near ambient temperature. Unprecedented 422 K beginning dehydrogenation temperature and up to 6.36 wt.% reliable hydrogen storage capacity are achieved. Fast hydrogen desorption is also provided by the system (5.49 wt.% in 1 h, 523 K). The in situ generated PdNi alloy clusters with suitable d-band centers are identified as the main active sites during the de/re-hydrogenation process by aberration-corrected transmission electron microscopy and theoretical simulations, while other active species including Pd/Ni pure phase clusters and Pd/Ni single atoms obtained via metallene ball milling, also enhance the reaction. These findings present fundamental insights into active species identification and rational design of highly efficient hydrogen storage materials.
Keyword ：
single atoms single atoms clusters clusters magnesium hydride magnesium hydride hydrogen storage materials hydrogen storage materials d-band center d-band center bilayer metallene bilayer metallene
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| GB/T 7714 | Xu, Nuo , Wang, Kaiwen , Zhu, Yunfeng et al. PdNi Biatomic Clusters from Metallene Unlock Record-Low Onset Dehydrogenation Temperature for Bulk-MgH2 [J]. | ADVANCED MATERIALS , 2023 , 35 (38) . |
| MLA | Xu, Nuo et al. "PdNi Biatomic Clusters from Metallene Unlock Record-Low Onset Dehydrogenation Temperature for Bulk-MgH2" . | ADVANCED MATERIALS 35 . 38 (2023) . |
| APA | Xu, Nuo , Wang, Kaiwen , Zhu, Yunfeng , Zhang, Yao . PdNi Biatomic Clusters from Metallene Unlock Record-Low Onset Dehydrogenation Temperature for Bulk-MgH2 . | ADVANCED MATERIALS , 2023 , 35 (38) . |
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Abstract ：
Dry reforming of methane (DRM) has been investigated for more than a century; the paramount stumbling block in its industrial application is the inevitable sintering of catalysts and excessive carbon emissions at high temperatures. However, the low-temperature DRM process still suffered from poor reactivity and severe catalyst deactivation from coking. Herein, we proposed a concept that highly durable DRM could be achieved at low temperatures via fabricating the active site integration with light irradiation. The active sites with Ni-O coordination (Ni-SA/CeO2) and Ni-Ni coordination (Ni-NP/CeO2) on CeO2, respectively, were successfully constructed to obtain two targeted reaction paths that produced the key intermediate (CH3O*) for anticoking during DRM. In particular, the operando diffuse reflectance infrared Fourier transform spectroscopy coupling with steady-state isotopic transient kinetic analysis (operando DRIFTS-SSITKA) was utilized and successfully tracked the anticoking paths during the DRM process. It was found that the path from CH3* to CH3O* over Ni-SA/CeO2 was the key path for anticoking. Furthermore, the targeted reaction path from CH3* to CH3O* was reinforced by light irradiation during the DRM process. Hence, the Ni-SA/CeO2 catalyst exhibits excellent stability with negligible carbon deposition for 230 h under thermo-photo catalytic DRM at a low temperature of 472 degrees C, while Ni-NP/CeO2 shows apparent coke deposition behavior after 0.5 h in solely thermal-driven DRM. The findings are vital as they provide critical insights into the simultaneous achievement of low-temperature and anticoking DRM process through distinguishing and directionally regulating the key intermediate species.
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| GB/T 7714 | Rao, Zhiqiang , Wang, Kaiwen , Cao, Yuehan et al. Light-Reinforced Key Intermediate for Anticoking To Boost Highly Durable Methane Dry Reforming over Single Atom Ni Active Sites on CeO2 [J]. | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY , 2023 , 145 (45) : 24625-24635 . |
| MLA | Rao, Zhiqiang et al. "Light-Reinforced Key Intermediate for Anticoking To Boost Highly Durable Methane Dry Reforming over Single Atom Ni Active Sites on CeO2" . | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 145 . 45 (2023) : 24625-24635 . |
| APA | Rao, Zhiqiang , Wang, Kaiwen , Cao, Yuehan , Feng, Yibo , Huang, Zeai , Chen, Yaolin et al. Light-Reinforced Key Intermediate for Anticoking To Boost Highly Durable Methane Dry Reforming over Single Atom Ni Active Sites on CeO2 . | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY , 2023 , 145 (45) , 24625-24635 . |
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Abstract ：
Single metal atoms decorated on earth-abundant transition-metal-based supports have attracted intensive attention toward oxygen evolution reaction (OER) due to their decent activity and low cost. However, further optimizing the catalytic performance is severely plagued by the limited active sites. Conventional optimization relies primarily on increasing the metal loading but is extremely difficult. Thus, it is imperative to go beyond the current design paradigms. Herein, it is reported that the anchored highly active single metal atoms can reinforce the electrochemical reconstruction of the supports and thus yield more substrate active sites. Consequently, increased amount of active sites and enhanced intrinsic activity can be readily realized simultaneously. Taking Ni2P4O12 decorated with single Ir atoms as a typical example, an extraordinary activity of eta 10 = 186 mV and eta 100 = 238 mV and robust stability up to 108 h are achieved. Mechanistic study uncovers that the reinforced reconstruction of Ni2P4O12 originates from the promoted PO43- leaching by single Ir atoms, which is an intrinsic feature of the supports to achieve such reinforcement. The proposed concept, decorating single metal atoms on supports featured by facile anion leaching, opens a new avenue to the design of practical electrocatalysts for efficient OER. Single Ir atoms decoration on Ni2P4O12 could enhance the intrinsic activity and reinforce the electrochemical reconstruction of the support to generate more active sites simultaneously. Comparison with Ir/NiO indicates the crucial role of supports with facile anion leaching in reinforcing electrochemical reconstruction. The Ir/Ni2P4O12 catalyst exhibits an extraordinary activity and robust stability for the oxygen evolution reaction.image
Keyword ：
enhanced reaction kinetics enhanced reaction kinetics reinforced electrochemical reconstruction reinforced electrochemical reconstruction oxygen evolution reaction oxygen evolution reaction single metal atom catalysts single metal atom catalysts facile anion leaching facile anion leaching
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| GB/T 7714 | Liu, Xue , Jing, Shaojie , Wang, Kaiwen et al. Double Bonuses Achieved in Single-Atom Catalysts for Efficient Oxygen Evolution: Enhanced Reaction Kinetics and Reinforced Electrochemical Reconstruction [J]. | ADVANCED FUNCTIONAL MATERIALS , 2023 . |
| MLA | Liu, Xue et al. "Double Bonuses Achieved in Single-Atom Catalysts for Efficient Oxygen Evolution: Enhanced Reaction Kinetics and Reinforced Electrochemical Reconstruction" . | ADVANCED FUNCTIONAL MATERIALS (2023) . |
| APA | Liu, Xue , Jing, Shaojie , Wang, Kaiwen , Ban, Chaogang , Ding, Junjie , Feng, Yajie et al. Double Bonuses Achieved in Single-Atom Catalysts for Efficient Oxygen Evolution: Enhanced Reaction Kinetics and Reinforced Electrochemical Reconstruction . | ADVANCED FUNCTIONAL MATERIALS , 2023 . |
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Abstract ：
Ultrasound-stimulated piezo-electrocatalysis has been studied for a period; however, the mechanism is still unclear mainly due to the coexistence with other multiple effects like sonocatalysis, which was usually ignored. In this work, with the non-piezoelectric H2Ti3O7 nanowires following the same experimental process in piezo-electrocatalysis, the sonocatalytic reduction performance of CO2 is investigated. By applying vibration under the excitation of ultrasound with various frequencies and powers, it is found that CO is the ultimate product with a selectivity of 100%, and the optimal CO yield of 8.3 mu mol g(-1) h(-1) is achieved with the addition of sacrificial agents. The H2Ti3O7 catalysts are also found to present a good recycling utilization ability. This work indicates that the sonocatalysis effect may exist in the piezo-electrocatalytic process using the ultrasonic excitation, which is suggested to be taken into consideration when exploring the mechanism of piezo-electrocatalysis in the future. Published under an exclusive license by AIP Publishing.
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| GB/T 7714 | Ma, Jiangping , Xiong, Xin , Ban, Chaogang et al. Ultrasound-triggered sonocatalytic reduction of CO2 via H2Ti3O7 nanowires [J]. | APPLIED PHYSICS LETTERS , 2022 , 121 (26) . |
| MLA | Ma, Jiangping et al. "Ultrasound-triggered sonocatalytic reduction of CO2 via H2Ti3O7 nanowires" . | APPLIED PHYSICS LETTERS 121 . 26 (2022) . |
| APA | Ma, Jiangping , Xiong, Xin , Ban, Chaogang , Wang, Kaiwen , Dai, Ji-Yan , Zhou, Xiaoyuan . Ultrasound-triggered sonocatalytic reduction of CO2 via H2Ti3O7 nanowires . | APPLIED PHYSICS LETTERS , 2022 , 121 (26) . |
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Abstract ：
MgH2 as one of potential solid-state hydrogen storage materials has been widely investigated during past decades due to its large capacity and abundant elemental reserves. Nonetheless, the presented ultra-high thermal stability and sluggish kinetics hinder a further application. In the present work, the Ni and Pt nano-clusters evolved from Ni@Pt core-shell nanoparticles facilitated the de/re-hydrogenation process of MgH2. The onset dehydrogenation temperature of MgH2-10 wt% Ni@Pt was greatly lowered by maximum 108 K compared with 601 K of the pristine MgH2, and the dehydrogenation process can be terminated below 573 K. The thermal stability of the MgH2-based system was remarkably tailored to 69.4 kJ (mol H-2)(-1) from 76.2 kJ (mol H-2)(-1) of the pristine MgH2. Meanwhile, the hydrogen storage kinetics of MgH2-10 wt% Ni@Pt was greatly improved compared with the pristine MgH2. Density functional theory calculations confirmed that Pt nano-clusters serving as a destabilizer and catalyst not only greatly destabilize the thermal stability of MgH2 but also catalyze its reactions, in particular with the Pt(2 2 0) slab. The effective catalyst-reactant interfaces coupling with regulated surface determined desorption/absorption were deeply investigated and built, leading to an excellent agreement with experiments. The involving of transition metal clusters lays foundation of a new way of improving the hydrogen storage properties and paves a way of developing next-generation hydrogen storage materials.
Keyword ：
Pt nano-clusters Pt nano-clusters MgH2 -based hydrogen storage materials MgH2 -based hydrogen storage materials Core-shell nanoparticles Core-shell nanoparticles De/re-hydrogenation kinetics De/re-hydrogenation kinetics Thermal stability Thermal stability
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| GB/T 7714 | Yuan, Zirui , Li, Shaohan , Wang, Kaiwen et al. in-situ formed Pt nano-clusters serving as destabilization-catalysis bi-functional additive for MgH2 [J]. | CHEMICAL ENGINEERING JOURNAL , 2022 , 435 . |
| MLA | Yuan, Zirui et al. "in-situ formed Pt nano-clusters serving as destabilization-catalysis bi-functional additive for MgH2" . | CHEMICAL ENGINEERING JOURNAL 435 (2022) . |
| APA | Yuan, Zirui , Li, Shaohan , Wang, Kaiwen , Xu, Nuo , Sun, Weiwei , Sun, Litao et al. in-situ formed Pt nano-clusters serving as destabilization-catalysis bi-functional additive for MgH2 . | CHEMICAL ENGINEERING JOURNAL , 2022 , 435 . |
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Abstract ：
Constructing dual sites is promising to break scaling relations between the adsorption energetics of reaction intermediates and ultimately improves the activity and selectivity due to the synergistic effect. However, it is a grand challenge to precisely form a dual-site configuration with one metal site adjacent to another active site. Loading single atoms onto oxides with pre-introduction of surface oxygen vacancies may be an alternative strategy to overcome such challenge. Motivated by our theoretical calculations that the dual sites formed by single Cu atoms and unsaturated Ti sites on TiO2 enables a higher activity towards hydrogen evolution from water splitting than corresponding single site, we successfully synthesized a Cu-1-Ti dual-site catalyst by depositing Cu single atoms on TiO2 nanoparticles with abundant surface oxygen vacancies. The designed target catalyst significantly outperforms the benchmark Pt nanoparticle decorated TiO2 with a high and stable activity towards photocatalytic hydrogen production.
Keyword ：
Cu atoms Cu atoms TiO2 TiO2 Dual single sites Dual single sites Photocatalyst hydrogen evolution Photocatalyst hydrogen evolution Single-atom catalysts Single-atom catalysts
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| GB/T 7714 | Feng, Yajie , Wang, Yang , Wang, Kaiwen et al. Constructing Cu-1-Ti dual sites for highly efficient photocatalytic hydrogen evolution [J]. | NANO ENERGY , 2022 , 103 . |
| MLA | Feng, Yajie et al. "Constructing Cu-1-Ti dual sites for highly efficient photocatalytic hydrogen evolution" . | NANO ENERGY 103 (2022) . |
| APA | Feng, Yajie , Wang, Yang , Wang, Kaiwen , Ban, Chaogang , Duan, Youyu , Meng, Jiazhi et al. Constructing Cu-1-Ti dual sites for highly efficient photocatalytic hydrogen evolution . | NANO ENERGY , 2022 , 103 . |
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Abstract ：
Recently, the bismuth-rich strategy via increasing the bismuth content has been becoming one of the most appealing approaches to improve the photocatalytic performance of bismuth oxyhalides. However, insights into the mechanism behind the encouraging experiments are missing. Herein, we report the results of the theory-led comprehensive picture of bismuth-rich strategy in bismuth oxyhalide photocatalysts, selecting Bi5O7X (X = F, Cl, Br, I) as a prototype. First-principle calculations revealed that the strategy enables good n-type conductivity, large intrinsic internal electric field, high photoreduction ability and outstanding harvest of visible light, and particularly ranked the intrinsic activity of this family: Bi5O7F > Bi5O7I > Bi5O7Br > Bi5O7Cl. Designed experiments confirmed the theoretical predictions, and together, these results are expected to aid future development of advanced photocatalysts.
Keyword ：
bismuth oxyhalides bismuth oxyhalides bismuth-rich strategy bismuth-rich strategy intrinsic activity intrinsic activity photocatalytic reduction photocatalytic reduction
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| GB/T 7714 | Wang, Yang , Meng, Jiazhi , Jing, Shaojie et al. Origin of Bismuth-Rich Strategy in Bismuth Oxyhalide Photocatalysts [J]. | ENERGY & ENVIRONMENTAL MATERIALS , 2022 , 6 (5) . |
| MLA | Wang, Yang et al. "Origin of Bismuth-Rich Strategy in Bismuth Oxyhalide Photocatalysts" . | ENERGY & ENVIRONMENTAL MATERIALS 6 . 5 (2022) . |
| APA | Wang, Yang , Meng, Jiazhi , Jing, Shaojie , Wang, Kaiwen , Ban, Chaogang , Feng, Yajie et al. Origin of Bismuth-Rich Strategy in Bismuth Oxyhalide Photocatalysts . | ENERGY & ENVIRONMENTAL MATERIALS , 2022 , 6 (5) . |
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Abstract ：
Surface-enhanced Raman spectroscopy (SERS) is an ultra-sensitive and rapid technique that is able to significantly enhance the Raman signals of analytes absorbed on functional substrates by orders of magnitude. Recently, semiconductor-based SERS substrates have shown rapid progress due to their great cost-effectiveness, stability and biocompatibility. In this work, three types of faceted Co3O4 microcrystals with dominantly exposed {100} facets, {111} facets and co-exposed {100}-{111} facets (denoted as C-100, C-111 and C-both, respectively) are utilized as SERS substrates to detect the rhodamine 6G (R6G) molecule and nucleic acids (adenine and cytosine). C-100 exhibited the highest SERS sensitivity among these samples, and the lowest detection limits (LODs) to R6G and adenine can reach 10(-7) M. First-principles density functional theory (DFT) simulations further unveiled a stronger photoinduced charge transfer (PICT) in C-100 than in C-111. This work provides new insights into the facet-dependent SERS for semiconductor materials.
Keyword ：
DFT simulation DFT simulation SERS SERS Co3O4 Co3O4 facet-dependent facet-dependent
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| GB/T 7714 | Feng, Yibo , Wang, Jiaxing , Hou, Jixiang et al. Facet-Dependent SERS Activity of Co3O4 [J]. | INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES , 2022 , 23 (24) . |
| MLA | Feng, Yibo et al. "Facet-Dependent SERS Activity of Co3O4" . | INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES 23 . 24 (2022) . |
| APA | Feng, Yibo , Wang, Jiaxing , Hou, Jixiang , Zhang, Xu , Gao, Yuhang , Wang, Kaiwen . Facet-Dependent SERS Activity of Co3O4 . | INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES , 2022 , 23 (24) . |
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Abstract ：
The conversion of CO2 into value-added chemicals through the electrocatalytic CO2 reduction reaction (CO2RR) is considered as an up-and-coming way to facilitate the renewable closed carbon cycle and energy storage. Therefore, the development of robust and low-cost CO2RR electrocatalysts is essential but challenging. Herein, a Ni single-atom catalyst (Ni-SAs-NC) was successfully prepared via a precursor assembly strategy and a subsequent one-step pyrolysis process. Characterization studies demonstrate that abundant Ni single-atom active sites with the coordination structure of Ni-N-4 are uniformly dispersed in Ni-SAs-NC, which consequently endow it with outstanding electrocatalytic CO2RR performance. Strikingly, the as-prepared Ni-SAs-NC can selectively convert CO2 into CO with a high faradaic efficiency of up to 98%, and can maintain the high values exceeding 90% in a wide potential range from -0.6 to -1.0 V. This work provides a new protocol to prepare high-efficiency but low-cost single-atom electrocatalysts toward the CO2RR and other electrochemical reactions.
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| GB/T 7714 | Wang, Wei-juan , Cao, Changsheng , Wang, Kaiwen et al. Boosting CO2 electroreduction to CO with abundant nickel single atom active sites dagger [J]. | INORGANIC CHEMISTRY FRONTIERS , 2021 , 8 (10) : 2542-2548 . |
| MLA | Wang, Wei-juan et al. "Boosting CO2 electroreduction to CO with abundant nickel single atom active sites dagger" . | INORGANIC CHEMISTRY FRONTIERS 8 . 10 (2021) : 2542-2548 . |
| APA | Wang, Wei-juan , Cao, Changsheng , Wang, Kaiwen , Zhou, Tianhua . Boosting CO2 electroreduction to CO with abundant nickel single atom active sites dagger . | INORGANIC CHEMISTRY FRONTIERS , 2021 , 8 (10) , 2542-2548 . |
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Abstract ：
High-valence cobalt sites are considered as highly active centers for the oxygen evolution reaction (OER) and their corresponding construction is thus of primary importance in the pursuit of outstanding performance. Herein, we report the design and facile synthesis of abundant high-valence cobalt sites by introducing Zn2+ into CoFe Prussian blue analogues (PBAs). The modification results in the drastic morphological transformation from a pure phase (CoFe-PBA) to a three-phase composite (CoFeZn-PBA), with a significant increase not only the amount of highly oxidized Co sites but the specific surface area (by up to 4 times). Moreover, the obtained sample also exhibits outstanding electric conductivity. Consequently, an excellent OER performance with an overpotential of 343 mV@10 mA cm(-2) and a Tafel slope of 75 mV dec(-1) was achieved in CoFeZn-PBA, which outperforms the commercial IrO2 catalyst. Further analysis reveals that CoFeZn-PBA becomes (oxyhydr)oxides after the OER.
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| GB/T 7714 | Zou, Hanjun , Liu, Xue , Wang, Kaiwen et al. Constructing highly active Co sites in Prussian blue analogues for boosting electrocatalytic water oxidation [J]. | CHEMICAL COMMUNICATIONS , 2021 , 57 (65) : 8011-8014 . |
| MLA | Zou, Hanjun et al. "Constructing highly active Co sites in Prussian blue analogues for boosting electrocatalytic water oxidation" . | CHEMICAL COMMUNICATIONS 57 . 65 (2021) : 8011-8014 . |
| APA | Zou, Hanjun , Liu, Xue , Wang, Kaiwen , Duan, Youyu , Wang, Cong , Zhang, Bin et al. Constructing highly active Co sites in Prussian blue analogues for boosting electrocatalytic water oxidation . | CHEMICAL COMMUNICATIONS , 2021 , 57 (65) , 8011-8014 . |
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