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学者姓名：程年才
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Abstract ：
Rational tailoring of the electronic structure at the defined active center of reconstructed metal (oxy)hydroxides (MOOH) during oxygen evolution reaction (OER) remains a challenge. With the guidance of density functional theory (DFT), herein a dual-site regulatory strategy is reported to tailor the d-band center of the Co site in CoOOH via the controlled electronic transfer at the RuOCoOFe bonding structure. Through the bridged O-2- site, electrons are vastly flowed from the t(2g)-orbital of the Ru site to the low-spin orbital of the Co site in the Ru-O-Co coordination and further transfer from the strong electron-electron repulsion of the Co site to the Fe site by the Co-O-Fe coordination, which balancing the electronic configuration of Co sites to weaken the over-strong adsorption energy barrier of OH* and O*, respectively. Benefiting from the highly active of the Co site, the constructed (Ru2Fe2Co6)OOH provide an extremely low overpotential of 248 mV and a Tafel slope of 32.5 mV dec-1 at 10 mA cm-2 accompanied by long durability in alkaline OER, far superior over the pristine and Co-O-Fe bridged CoOOH catalysts. This work provides guidance for the rational design and in-depth analysis of the optimized role of metal dual-sites.
Keyword ：
dual-sites dual-sites electronic structures electronic structures metal (oxy)hydroxides metal (oxy)hydroxides oxygen adsorption energetics oxygen adsorption energetics oxygen evolution reactions oxygen evolution reactions
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| GB/T 7714 | Zhu, Yu , Zhang, Shunqiang , Chen, Runzhe et al. Controllable Electronic Transfer Tailoring d-band Center via Cobalt-Oxygen-Bridged Ru/Fe Dual-sites for Boosted Oxygen Evolution [J]. | SMALL , 2024 . |
| MLA | Zhu, Yu et al. "Controllable Electronic Transfer Tailoring d-band Center via Cobalt-Oxygen-Bridged Ru/Fe Dual-sites for Boosted Oxygen Evolution" . | SMALL (2024) . |
| APA | Zhu, Yu , Zhang, Shunqiang , Chen, Runzhe , Wang, Zichen , Wu, Wei , Jiang, Haoran et al. Controllable Electronic Transfer Tailoring d-band Center via Cobalt-Oxygen-Bridged Ru/Fe Dual-sites for Boosted Oxygen Evolution . | SMALL , 2024 . |
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Ru-based materials are promising electrocatalysts for hydrogen evolution reaction (HER) owing to their low-cost (one twenty-fifth of Pt) and similar Gibbs free energy of H* adsorption (AGH*) to that of Pt. However, the inadequate ability for the water dissociation of Ru catalysts is significantly impeding the water splitting efficiency. In this work, we demonstrate an atomically ordered hexagonal Ru-Ni alloy with compressive-strained Ru skin as a high-performance HER catalyst for significantly boosting the water dissociation. The Ordered Ru-Ni achieves an optimized catalytic activity for alkaline HER with a low overpotential of 23 mV at 10 mA cm-2, Tafel slope of 25.9 mV dec-1 and superior mass activity of 4.83 A mg-Ru1, which is 15.1 times higher than Ru/C. According to DFT calculations, the ordered RuNi core imposes homogeneous compressive strain on the Ru skin, resulting in an optimum binding energy towards H*/OH* intermediates on Ru active sites for rapid Tafel step kinetics. Moreover, the decreased H2O dissociation energy barrier of Ordered Ru-Ni suggests a promoted VolmerTafel kinetics is achieved, significantly boosting the overall HER efficiency. This work provides a practical avenue for surface strain engineering of Ru-based catalysts to promote the HER activity.
Keyword ：
Compressive strain Compressive strain Hydrogen evolution reaction Hydrogen evolution reaction Ru-Ni alloy Ru-Ni alloy Ru shell Ru shell Water dissociation Water dissociation
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| GB/T 7714 | Chen, Xuwen , Ye, Lifan , Wu, Wei et al. Compressed Ru skin on atomic-ordered hexagonal Ru-Ni enabling rapid Volmer-Tafel kinetics for efficient alkaline hydrogen evolution [J]. | CHEMICAL ENGINEERING JOURNAL , 2024 , 487 . |
| MLA | Chen, Xuwen et al. "Compressed Ru skin on atomic-ordered hexagonal Ru-Ni enabling rapid Volmer-Tafel kinetics for efficient alkaline hydrogen evolution" . | CHEMICAL ENGINEERING JOURNAL 487 (2024) . |
| APA | Chen, Xuwen , Ye, Lifan , Wu, Wei , Chen, Suhao , Wang, Zichen , Zhu, Yu et al. Compressed Ru skin on atomic-ordered hexagonal Ru-Ni enabling rapid Volmer-Tafel kinetics for efficient alkaline hydrogen evolution . | CHEMICAL ENGINEERING JOURNAL , 2024 , 487 . |
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Precisely controlling the strain of Pt-based intermetallic to ensure high performance and stability is a massive task for sustainable proton-exchange-membrane-fuel-cells. Herein, the Al single-atom was trapped into the L12-Pt3Co intermetallic core to precisely tailor the strain state on the Pt-skin for fast oxygen reduction reaction kinetics. Theoretical calculations firstly predicted that only tailored tension can accelerate the protonation of O2 on L12-Pt3Co@Pt without creating an additional energy barrier for subsequent oxygen-containing intermediates desorption. Experimentally, Al single-atom confined in the L12-Pt3Co lattice by substituting partial Co occupancy, imposing tailored ∼ 0.2 % tension on Pt-skin compared to the L12-Pt3Co. L12-Al-Pt3Co@Pt/C exhibits enhanced mass activity which is ten-time improvement over commercial Pt/C. More significantly, XAS and DFT results reveal that the Al single-atom can strengthen the Pt-Co bonding, enhancing the stability of L12-Al-Pt3Co@Pt/C in oxygen reduction. This work provides an avenue to design the strain by single-atom for sustainable energy conversion technologies. © 2024 Elsevier B.V.
Keyword ：
Aluminum Aluminum Atomic layer deposition Atomic layer deposition Atoms Atoms Binary alloys Binary alloys Cobalt alloys Cobalt alloys Design for testability Design for testability Electrolytic reduction Electrolytic reduction Intermetallics Intermetallics Oxygen Oxygen Platinum alloys Platinum alloys Proton exchange membrane fuel cells (PEMFC) Proton exchange membrane fuel cells (PEMFC) Reaction kinetics Reaction kinetics
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| GB/T 7714 | Wu, Wei , Qu, Wei , Wang, Zichen et al. Single-atom Al precisely modulate the strain of Pt3Co intermetallic for superior oxygen catalytic performance [J]. | Chemical Engineering Journal , 2024 , 491 . |
| MLA | Wu, Wei et al. "Single-atom Al precisely modulate the strain of Pt3Co intermetallic for superior oxygen catalytic performance" . | Chemical Engineering Journal 491 (2024) . |
| APA | Wu, Wei , Qu, Wei , Wang, Zichen , Tan, Yangyang , Chen, Runzhe , Chen, Suhao et al. Single-atom Al precisely modulate the strain of Pt3Co intermetallic for superior oxygen catalytic performance . | Chemical Engineering Journal , 2024 , 491 . |
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For the most commonly applied platinum-based catalysts of direct methanol fuel cells, the adsorption ability toward reaction intermediates, including CO and OH, plays a vital role in their catalytic activity and antipoisoning in anodic methanol oxidation reaction (MOR). Herein, guided by a theoretical mechanism study, a favorable modulation of the electronic structure and intermediate adsorption energetics for Pt active sites is achieved by constructing the triple-phase interfacial structure between tin oxide (SnO2), platinum (Pt), and nitrogen-doped graphene (NG). From the strong electronic exchange at the triple-phase interface, the adsorption ability toward MOR reaction intermediates on Pt sites could be efficiently optimized, which not only inhibits the adsorption of CO* on active sites but also facilitates the adsorption of OH* to strip the poisoning species from the catalyst surface. Accordingly, the resulting catalyst delivers excellent catalytic activity and antipoisoning ability for MOR catalysis. The mass activity reaches 1098 mA mg(Pt)(-1), 3.23 times of commercial Pt/C. Meanwhile, the initial potentials and main peak for CO oxidation are also located at a much lower potential (0.51 and 0.74 V) against commercial Pt/C (0.83 and 0.89 V).
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| GB/T 7714 | Chen, Runzhe , Wang, Zichen , Chen, Suhao et al. Optimizing Intermediate Adsorption on Pt Sites via Triple-Phase Interface Electronic Exchange for Methanol Oxidation [J]. | INORGANIC CHEMISTRY , 2024 , 63 (9) : 4364-4372 . |
| MLA | Chen, Runzhe et al. "Optimizing Intermediate Adsorption on Pt Sites via Triple-Phase Interface Electronic Exchange for Methanol Oxidation" . | INORGANIC CHEMISTRY 63 . 9 (2024) : 4364-4372 . |
| APA | Chen, Runzhe , Wang, Zichen , Chen, Suhao , Wang, Liang , Wu, Wei , Zhu, Yu et al. Optimizing Intermediate Adsorption on Pt Sites via Triple-Phase Interface Electronic Exchange for Methanol Oxidation . | INORGANIC CHEMISTRY , 2024 , 63 (9) , 4364-4372 . |
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The transformation of Li2S2 -Li2S is indubitably the most crucial and labored rate -limiting step among the sophisticated reactions for the lithium -sulfur batteries (LSBs), the adjustment of which is anticipated to impede the shuttle effect. Herein, a N, Se dual -doped carbon nanocages embedded by Co-CoSe2 nanoparticles (Co-CoSe2 @NSeC) is employed as a functional coating layer on commercial separator to improve the performance of LSBs. The well -designed N, Se co -doped nanostructures endow the modified layer with a satisfactory capacity for blocking polysulfides. Both calculations and experiments jointly disclose that the Li2S2 to Li2S reaction, including the liquid -solid conversion, was prominently expedited both thermodynamically and electrodynamically. Consequently, the batteries fabricated with Co-CoSe2 @NSeC modified separator can deliver a favorable 764.2 mAh g-1 with 8.0 C, accompanied by a salient long cycling lifespan (only 0.066 % at 1 C and 0.061 % under 2 C after 10 0 0 and 20 0 0 cycles), and a desired anode protection. In addition, despite a raised areal loading of 7.53 mg cm-2 was introduced, the cells assembled by Co-CoSe2 @NSeC@PP are allowed to produce an outstanding initial behavior of 8.71 mAh cm-2 under 0.2 C. This work may reinforce further explorations and serve with valuable insights into N, Se dual -doping materials for high-performance LSBs. (c) 2024 Published by Elsevier Ltd on behalf of The editorial office of Journal of Materials Science & Technology.
Keyword ：
Hollow nanostructure Hollow nanostructure Li2 S2-Li2 S phase-transition Li2 S2-Li2 S phase-transition Lithium-sulfur batteries Lithium-sulfur batteries Modified separator Modified separator N Se doping carbon N Se doping carbon
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| GB/T 7714 | Zheng, Ming , Wu, Wei , Luo, Ruijian et al. Constructing stronger interaction with polysulfides for faster conversion of Li2S2 to Li2S by Co-CoSe2 @N, Se-doped carbon nanocages in lithium-sulfur batteries [J]. | JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY , 2024 , 195 : 165-176 . |
| MLA | Zheng, Ming et al. "Constructing stronger interaction with polysulfides for faster conversion of Li2S2 to Li2S by Co-CoSe2 @N, Se-doped carbon nanocages in lithium-sulfur batteries" . | JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY 195 (2024) : 165-176 . |
| APA | Zheng, Ming , Wu, Wei , Luo, Ruijian , Chen, Suhao , Zhao, Junzhe , Cheng, Niancai . Constructing stronger interaction with polysulfides for faster conversion of Li2S2 to Li2S by Co-CoSe2 @N, Se-doped carbon nanocages in lithium-sulfur batteries . | JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY , 2024 , 195 , 165-176 . |
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The insufficient durability of Pt-based catalysts and the sluggish kinetics of oxygen reduction reaction (ORR) is hampering the development of proton exchange membrane fuel cells (PEMFCs) for commercialization. Herein, a single atom Ti-modified activated nitrogen-doped porous carbon (Ti-a-NPC) is designed to equalize O2-activation/*OH-removal through regulating the charge rearrangement of ultra-small L12-Pt3Co for efficient and durable oxygen reduction. The Ti single-atom modified in the surface/pore of Ti-a-NPC can anchor the Pt-based intermetallic nanoparticles (NPs) not only guarantees Pt-based intermetallics' ultra-fine size (approximate to 2.62 nm) but also maintains Pt-based intermetallics during ORR process. The enhanced catalyst (L12-Pt3Co/Ti-a-NPC) achieves 11-fold mass activity (1.765 A mgPt-1) compared to commercial Pt/C. Notably, after 30 000 cycles of accelerated durability tests, the mass activity of the L12-Pt3Co/Ti-a-NPC only decreased by 3.7%, while that of commercial Pt/C decreased by 37.1%. Rationalized by theoretical simulation, the introduction of Ti atoms can form charge channels between L12-Pt3Co NPs and Ti-a-NPC, accelerating the charge transfer in the ORR process. Furthermore, the charge of L12-Pt3Co will accumulate to Ti atoms and buffer the electron transfer of L12-Pt3Co to the N atoms, thus optimizing the adsorption performance of the active site to the oxygen-containing intermediate and improving the intrinsic activity of the catalyst. The single-atom Ti synergizes with the confinement effect of Ti-a-NPC not only restricting the size increase of Pt-based intermetallics during the ordering process (average size 2.6 nm) but also inhibiting the shedding and migration of Pt-based intermetallics under fuel cell operating conditions. The charge of ultra-small L12-Pt3Co is regulated by single atom Ti to equalize O2-activation/*OH-removal for efficient oxygen reduction. image
Keyword ：
charge rearrangement charge rearrangement fuel cells fuel cells oxygen reduction reaction oxygen reduction reaction Pt-based intermetallics Pt-based intermetallics Ti single-atom Ti single-atom
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| GB/T 7714 | Wang, Zichen , Wu, Wei , Jiang, Haoran et al. Ti Single Atom Enhancing Pt-Based Intermetallics for Efficient and Durable Oxygen Reduction [J]. | ADVANCED FUNCTIONAL MATERIALS , 2024 . |
| MLA | Wang, Zichen et al. "Ti Single Atom Enhancing Pt-Based Intermetallics for Efficient and Durable Oxygen Reduction" . | ADVANCED FUNCTIONAL MATERIALS (2024) . |
| APA | Wang, Zichen , Wu, Wei , Jiang, Haoran , Chen, Suhao , Chen, Runzhe , Zhu, Yu et al. Ti Single Atom Enhancing Pt-Based Intermetallics for Efficient and Durable Oxygen Reduction . | ADVANCED FUNCTIONAL MATERIALS , 2024 . |
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The exploitation of durable and highly active Pt-based electrocatalysts for the oxygen reduction reaction (ORR) is essential for the commercialization of proton exchange membrane fuel cells (PEMFCs). Herein, we designed Pt@Pt 3 Ti core-shell nanoparticles with atomic-controllable shells through precise thermal diffusing Ti into Pt nanoparticles for effective and durable ORR. Combining theoretical and experiment analysis, we found that the lattice strain of Pt 3 Ti shells can be tailored by precisely controlling the thickness of Pt 3 Ti shell in atomic-scale on account of the lattice constant difference between Pt and Pt 3 Ti to optimize adsorption properties of Pt 3 Ti for ORR intermediates, thus enhancing its performance. The Pt@Pt 3 Ti catalyst with one-atomic Pt 3 Ti shell (Pt@1L-Pt 3 Ti/TiO 2 -C) demonstrates excellent performance with mass activity of 592 mA mg Pt -1 and durability nearly 19.5-fold that of commercial Pt/C with negligible decay (2 %) after 30,0 0 0 potential cycles (0.6-1.0 V vs. RHE). Notably, at higher potential cycles (1.0 V-1.5 V vs. RHE), Pt@1L-Pt 3 Ti/TiO 2 -C also showed far superior durability than Pt/C (9.6 % decayed while 54.8 % for commercial Pt/C). This excellent stability is derived from the intrinsic stability of Pt 3 Ti alloy and the confinement effect of TiO 2 -C. The catalyst's enhancement was further confirmed in PEMFC configuration. (c) 2024 Published by Elsevier Ltd on behalf of The editorial office of Journal of Materials Science & Technology.
Keyword ：
Atomic controllable Atomic controllable Compressive strain Compressive strain Core-shell structure Core-shell structure Oxygen reduction reaction Oxygen reduction reaction Pt-based catalysts Pt-based catalysts
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| GB/T 7714 | Jiang, Haoran , Wang, Zichen , Chen, Suhao et al. Atomic controlled shell thickness on Pt@Pt 3 Ti core-shell nanoparticles for efficient and durable oxygen reduction [J]. | JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY , 2024 , 205 : 212-220 . |
| MLA | Jiang, Haoran et al. "Atomic controlled shell thickness on Pt@Pt 3 Ti core-shell nanoparticles for efficient and durable oxygen reduction" . | JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY 205 (2024) : 212-220 . |
| APA | Jiang, Haoran , Wang, Zichen , Chen, Suhao , Xiao, Yong , Zhu, Yu , Wu, Wei et al. Atomic controlled shell thickness on Pt@Pt 3 Ti core-shell nanoparticles for efficient and durable oxygen reduction . | JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY , 2024 , 205 , 212-220 . |
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Modulating the electronic configuration of the substrate to achieve the optimal chemisorption toward polysulfides (LiPSs) for boosting polysulfide conversion is a promising way to the efficient Li-S batteries but filled with challenges. Herein, a Co/CoS2 heterostructure is elaborately built to tuning d-orbital electronic structure of CoS2 for a high-performance electrocatalyst. Theoretical simulations first evidence that Co metal as the electron donator can form a built-in electric field with CoS2 and downshift the d-band center, leading to the well-optimized adsorption strength for lithium polysulfides on CoS2, thus contributing a favorable way for expediting the redox reaction kinetics of LiPSs. As verification of prediction, a Co/CoS2 heterostructure implanted in porous hollow N, S co-doped carbon nanocage (Co/CoS2@NSC) is designed to realize the electronic configuration regulation and promote the electrochemical performance. Consequently, the batteries assembled with Co/CoS2@NSC cathode display an outstanding specific capacity and an admirable cycling property as well as a salient property of 8.25 mAh cm(-2) under 8.18 mg cm(-2). The DFT calculation also reveals the synergistic effect of N, S co-doping for enhancing polysulfide adsorption as well as the detriment of excessive sulfur doping.
Keyword ：
Co/CoS2 heterojunction Co/CoS2 heterojunction hollow structures hollow structures lithium-sulfur batteries lithium-sulfur batteries N,S co-doping N,S co-doping
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| GB/T 7714 | Zheng, Ming , Zhao, Junzhe , Wu, Wei et al. Co/CoS2 Heterojunction Embedded in N, S-Doped Hollow Nanocage for Enhanced Polysulfides Conversion in High-Performance Lithium-Sulfur Batteries [J]. | SMALL , 2023 , 20 (3) . |
| MLA | Zheng, Ming et al. "Co/CoS2 Heterojunction Embedded in N, S-Doped Hollow Nanocage for Enhanced Polysulfides Conversion in High-Performance Lithium-Sulfur Batteries" . | SMALL 20 . 3 (2023) . |
| APA | Zheng, Ming , Zhao, Junzhe , Wu, Wei , Chen, Runzhe , Chen, Suhao , Cheng, Niancai . Co/CoS2 Heterojunction Embedded in N, S-Doped Hollow Nanocage for Enhanced Polysulfides Conversion in High-Performance Lithium-Sulfur Batteries . | SMALL , 2023 , 20 (3) . |
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Spineloxides, representing an emerging class of highly activecatalysts for oxygen evolution (OER), suffer from weak covalency ofmetal d and oxygen p orbitals from their typical crystal structure,which generally proceeds the OER with an adsorbate evolution mechanism(AEM) pathway. For activating the lattice oxygen in spinel oxidesto bypass the scaling relationship limitation of AEM, we herein growthe sulfate salts on the octahedral sites of spinel NiFe2O4 to introduce the Ni4+ cations and Ni vacanciesin octahedral sites, which exhibit remarkable OER performance withan overpotential of 293 mV at 500 mA cm(-2). Experimentsand theoretical calculations reveal that the formation Ni4+ cations and Ni vacancies jointly enhance the metal-oxygenhybridization and strengthen the metal-oxygen bond covalencyin both NiFe2O4 and NiFeOOH phases, activatingthe lattice oxygen and successfully triggering the lattice oxygenmechanism (LOM) pathway on spinel oxides.
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| GB/T 7714 | Chen, Runzhe , Wang, Zichen , Chen, Suhao et al. Activating Lattice Oxygen in Spinel Oxides via Engineering Octahedral Sites for Oxygen Evolution [J]. | ACS ENERGY LETTERS , 2023 , 8 (8) : 3504-3511 . |
| MLA | Chen, Runzhe et al. "Activating Lattice Oxygen in Spinel Oxides via Engineering Octahedral Sites for Oxygen Evolution" . | ACS ENERGY LETTERS 8 . 8 (2023) : 3504-3511 . |
| APA | Chen, Runzhe , Wang, Zichen , Chen, Suhao , Wu, Wei , Zhu, Yu , Zhong, Jun et al. Activating Lattice Oxygen in Spinel Oxides via Engineering Octahedral Sites for Oxygen Evolution . | ACS ENERGY LETTERS , 2023 , 8 (8) , 3504-3511 . |
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Pt-based nanoclusters toward the hydrogen evolution reaction (HER) remain the most promising electrocatalysts. However, the sluggish alkaline Volmer-step kinetics and the high-cost have hampered progress in developing high-performance HER catalysts. Herein, we propose to construct sub-nanometer NiO to tune the d-orbital electronic structure of nanocluster-level Pt for breaking the Volmer-step limitation and reducing the Pt-loading. Theoretical simulations firstly suggest that electron transfer from NiO to Pt nanoclusters could downshift the Ed-band of Pt and result in the well-optimized adsorption/desorption strength of the hydrogen intermediate (H*), therefore accelerating the hydrogen generation rate. NiO and Pt nanoclusters confined into the inherent pores of N-doped carbon derived from ZIF-8 (Pt/NiO/NPC) were designed to realize the structure of computational prediction and boost the alkaline hydrogen evolution. The optimal 1.5%Pt/NiO/NPC exhibited an excellent HER performance and stability with a low Tafel slope (only 22.5 mv dec(-1)) and an overpotential of 25.2 mV at 10 mA cm(-2). Importantly, the 1.5%Pt/NiO/NPC possesses a mass activity of 17.37 A mg(-1) at the overpotential of 20 mV, over 54 times higher than the benchmark 20 wt% Pt/C. Furthermore, DFT calculations illustrate that the Volmer-step could be accelerated owing to the high OH- attraction of NiO nanoclusters, leading to the Pt nanoclusters exhibiting a balance of H* adsorption and desorption (Delta G(H*) = -0.082 eV). Our findings provide new insights into breaking the water dissociation limit of Pt-based catalysts by coupling with a metal oxide.
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| GB/T 7714 | Guo, Fei , Zhang, Zeyi , Chen, Runzhe et al. Dual roles of sub-nanometer NiO in alkaline hydrogen evolution reaction: breaking the Volmer limitation and optimizing d-orbital electronic configuration [J]. | MATERIALS HORIZONS , 2023 , 10 (8) : 2913-2920 . |
| MLA | Guo, Fei et al. "Dual roles of sub-nanometer NiO in alkaline hydrogen evolution reaction: breaking the Volmer limitation and optimizing d-orbital electronic configuration" . | MATERIALS HORIZONS 10 . 8 (2023) : 2913-2920 . |
| APA | Guo, Fei , Zhang, Zeyi , Chen, Runzhe , Tan, Yangyang , Wu, Wei , Wang, Zichen et al. Dual roles of sub-nanometer NiO in alkaline hydrogen evolution reaction: breaking the Volmer limitation and optimizing d-orbital electronic configuration . | MATERIALS HORIZONS , 2023 , 10 (8) , 2913-2920 . |
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