FUEL
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2025
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IF 7.5
Yanan Ma,Dingyu Zhang,Haimeng Wang,Yuxuan Liang,Yuan Zhang,Fengfeng Yan,Liang Sun,Qian Wang,Wei Li
Synthesis of multiple-site single-atom catalyst (SAC) with metal-containing nanoparticles by using zeolite imidazole framework (ZIF) for improving the bifunctional electrocatalytic performance is of great significance, yet it is also a challenge. Trimetallic ZIF-derived porous carbon nanosheets with the CoFe alloy nanoparticles enclosed in nitrogen-doped carbon nanotubes (N-CNTs) are fabricated by utilizing three transition metals as ZIF precursors and sodium chloride as templates via a typical two-step process, including synthesis and pyrolysis. By building CoFe alloy and tailoring d-band center ( E d ) of the Co site, the as-obtained FeCoZn@S-CN ZIF exhibits predominant kinetic activity and durability towards ORR and OER with an extremely low potential gap (Δ E ) value of 0.584 V, exceeding many other efficient counterparts. This study provides an effective approach for designing and synthesizing atomically dispersed multi-metal site catalysts with alloyed nanoparticles to achieve high-efficient bifunctional electrocatalytic performance in the application of the recharged zinc-air battery (ZAB).
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
·
IF 9.4
Zhiliang Jin,Cheng Yang
The research in the field of photocatalysis has progressed, with the development of heterojunctions being recognized as an effective method to improve carrier separation efficiency in light-induced processes. In this particular study, CuCo 2 S 4 particles were attached to a new cubic CdS surface to create an S-scheme heterojunction, thus successfully addressing this issue. Specifically, owing to the higher conduction band and Fermi level of CuCo 2 S 4 compared to CdS, they serve as the foundation and driving force for the formation of an S-scheme heterojunction. Through in-situ X-ray photoelectron spectroscopy and electron paramagnetic resonance analysis, the direction of charge transfer in the composite photocatalyst under light exposure was determined, confirming the charge transfer mechanism of the S-scheme heterojunction. By effectively constructing the S-scheme heterojunction, the d-band center of the composite photocatalyst was adjusted, reducing the energy needed for electron filling in the anti-bonding energy band, promoting the transfer of photogenerated carriers, and ultimately enhancing the photocatalytic hydrogen production . performance. After optimization, the hydrogen evolution activity of the composite photocatalyst CdS-C/CuCo 2 S 4 -3 reached 5818.9 μmol g −1 h −1 , which is 2.6 times higher than that of cubic CdS (2272.3 μmol g −1 h −1 ) and 327.4 times higher than that of CuCo 2 S 4 (17.8 μmol g −1 h −1 ), showcasing exceptional photocatalytic activity. Electron paramagnetic resonance and in situ X-ray photoelectron spectroscopy have established a theoretical basis for designing and constructing S-scheme heterojunctions, offering a viable method for adjusting the D-band center to enhance the performance of photocatalytic hydrogen evolution.
研究领域:
材料科学
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能源化学
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环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
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2025
·
IF 14.3
Xianyu Chu,Yanan Wang,Li Jing,Wei Jiang,Yuanyuan Wu,Ming Lu,Bo Liu,Chunbo Liu,Yantao Sun,Guangbo Che
Constructing heterostructures to regulate the electronic structure is an effective strategy for enhancing the oxygen evolution reaction (OER) electrocatalytic activity. Herein, we prepared heterostructured Co 4 S 3 /CoP 3 (CoPS/NFF) electrocatalysts through a one-step phosphorization and sulfuration process. The synthesized electrode drives an overpotential of 190, 272, and 331 mV at 20, 50, and 100 mA cm −2 for OER in 1 M KOH alkaline media, respectively. These values outperformed those of monophase Co 4 S 3 and CoP 3 as well as the majority of transition metal-based catalysts previously reported. Furthermore, the Density Functional Theory (DFT) calculation results show that charge redistribution occurs at CoPS/NFF heterogeneous interfaces, which facilitates charge transfer and improves catalytic activity. The CoPS/NFF with heterostructure optimizes the adsorption strength of oxygen-containing intermediates (*O, *OH, and *OOH) by appropriately adjusting the d-band center energy level, thereby reducing the energy barrier of OER. This work provides a new perspective on rational design strategies for efficient transition metal-based electrocatalysts by inducing d-band center regulation through the construction of heterostructures.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
·
IF 21.1
Su Li,Jinkai Qiu,Zijun Bian,Bin Shao,Zhicheng Liu,Cheng Lian,Honglai Liu,Jun Hu
The dry reforming of carbonate with methane (CaDRM) can be one of the breakthrough technologies to address the challenge of mitigating inevitable CO 2 emissions into value-added chemicals but remains great challenges for efficient catalysts design. In this study, we break the trade-off between the catalytic activity and the carbon deposit by tailoring the d-band center of Ni through Fe doping, which matches the energy level of CH 4 * dehydrogenation but is far away from that of the over cleavage of CH* . In this light, the porous spherical Fe x Ni/Al 2 O 3 catalysts with Ni 3 Fe alloy nanoaggregates are obtained through a one-step spray drying method. The optimized Fe 0.6 Ni/Al 2 O 3 catalyst shows an excellent catalytic activity with a superior CO selectivity of 91.75 % at a complete CaCO 3 conversion at 700°C, and successfully prevents the carbon deposit to maintain its excellent stability. Moreover, the extremely low activation energy of 45.2 kJ/mol and the good porosity of Fe x Ni/Al 2 O 3 ensure its fast dynamics. Therefore, this tailoring d-band center approach through the formation of alloy catalysts supplied a novel strategy for effectively cracking hydrogen species while avoiding over cleavage of CH x * in the thermal catalysis, which promoted the CaDRM technology to be a promising solution for carbon neutrality in industrial sectors in near future.
研究领域:
化学工程
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Nanoscale
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2025
·
IF 5.1
Bo Li,Lipan Luo,Yujia Liu,Xiaohan Zhou,Yuyu Zhang,Lishuai Song,Nan Liu,Qing Tang,Zequan Li
Pt/TiO2 photocatalysts were synthesized using incipient wetness impregnation followed by oxidative and/or reductive thermal treatments. The loading dimensions of Pt elements on the TiO2 surface (PtP, PtSA, and PtC) were controlled by varying the impregnated solution. Experimental results demonstrate that PtC with intermediate size exhibits the highest photolysis rate under 300W xenon lamp irradiation, achieving a hydrogen yield of 11.42 mmol g^-1 h^-1 and an apparent quantum yield of 40.65%. Similarly, Ru/TiO2 and Ir/TiO2 photocatalysts prepared under the same conditions exhibited the same pattern. Photoelectrochemical tests reveal that PtC/TiO2 has the narrowest band gap, the highest interfacial charge transfer capacity, and the greatest carrier separation efficiency. DFT calculations indicate that PtC/TiO2 has the most suitable d-band center, resulting in a close-to-zero ΔGH* value of 0.05 eV. This optimal value significantly balances the adsorption and desorption of hydrogen intermediates (H*) during the photocatalytic hydrogen evolution (PHE) reaction. This study provides new insights into the preparation of precious metal-loaded photocatalysts.
研究领域:
材料科学
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能源化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
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2025
·
IF 8.2
Fengyu Zhang,Yanping Yang,Qian Wang,Xiaomeng Chen,Lulu Xie,Xintao Li,Dianqing Li,Junting Feng,Xue Duan
When single-atom catalysts are oriented toward practical applications, in addition to balancing the seesaw between activity and selectivity, the capability of thermal management also merits attention. Herein, we proposed a facility approach that, based on active Pd in the state of a single atom, tunes the guest Cu size to simultaneously enhance the effect of d-electron domination and the heat transfer behavior in microregions. Along with the Cu size in an order of magnitude increase, more delocalized electrons were generated and transferred to isolated Pd sites, with the d band center shifting from 1.438 to 1.052 eV, closer to the Fermi level. Simultaneously, more long-range ordered lattices are much favorable for transferring in situ generated thermally phonons with the diffusivity surging from 12.36 to 103.49 mm2/s. The optimized Pd1Cu-SAA catalyst exhibited state-of-the-art performance in acetylene hydrogenation, achieving full conversion at 140 °C, with 95.3% selectivity and good stability in the test period.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
·
IF 9.4
Yuci Xin,Yong Wu,Xingan Dong,Yuhan Li,Zhenxiang Cheng,Jianli Wang,Xiaolong Guo,Peng Yu
Amorphous electrocatalysts display several unique advantages in electricity-driven water splitting compared to their crystalline analogs, but understanding their structure–activity relationships remains a major challenge. Herein, we show that the d- and p-electronic states of amorphous Ni-Fe-B can be subtly manipulated by varying the Ni and Fe contents. The optimal Ni-Fe-B alloy exhibits a high performance in the oxygen evolution reaction (OER), as supported by its impressive stability (no clear degradation after 100 h) and considerably lower overpotential compared to those of its crystalline analogs. Based on theoretical calculations, different Ni and Fe contents can cause significant shifts in the d-band levels of Ni and Fe and the p-band level of B, thus altering the OER activity. Additionally, the energy difference between the d- and p-band centers (ΔE ad-p ) may be an effective index for use in reflecting the structure–activity relationship of an amorphous Ni-Fe-B alloy in the OER. An amorphous Ni-Fe-B alloy with a smaller ΔE ad-p displays a higher intrinsic activity. This study supplies a unique direction for use in constructing the structure–activity relationships of amorphous electrocatalysts by revealing the role of ΔE ad-p , which promotes fundamental research and the practical application of amorphous electrocatalysts.
研究领域:
材料科学
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电催化
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理论计算
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Dandan Zhu,Meijuan Chen,Yu Huang,Rong Li,Tingting Huang,Jun-ji Cao,Zhenxing Shen,Shun Cheng Lee
Formaldehyde is a typical indoor air pollutant that has posed severely adverse effects on human health. Herein, a novel FeCo alloy nanoparticle-embedded nitrogen-doped carbon (FeCo@NC) was synthesized with the aim of tailoring the transition-metal d-band structure toward an improved formaldehyde oxidation activity for the first time. A unique core@shell metal–organic frameworks (MOFs) architecture with a Fe-based Prussian blue analogue core and Co-containing zeolite imidazole framework shell was firstly fabricated. Then, Fe and Co ion alloying was readily achieved owing to the inherent MOF porosity and interionic nonequilibrium diffusion occurring during pyrolysis . High-angle annular dark-field scanning transmission electron microscopy and X-ray absorption fine structure spectra confirm that small FeCo alloys in situ form in FeCo@NC, which exhibits a higher formaldehyde removal efficiency (93%) than the monometallic Fe-based catalyst and a remarkable CO 2 selectivity (85%) at room temperature. Density functional theory calculations indicate the number of electrons transferred from the metal core to the outer carbon layer is altered by alloying Fe and Co. More importantly, a downshift in the d-band center relative to the Fermi level occurs from − 0.93 to − 1.04 eV after introducing Co, which could alleviate the adsorption of reaction intermediates and greatly improve the catalytic performance.
研究领域:
环境科学
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材料科学
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化学
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2025
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IF 8.3
Shaorou Ke,Yajing Zhao,Xin Min,Xinyu Zhu,Xin Li,Bozhi Yang,Fan Yang,Xiaowen Wu,Ruiyu Mi,Yangai Liu,Zhaohui Huang,Minghao Fang
Platinum-based bimetallic catalysts exhibit superior hydrogen evolution reaction performance compared to single platinum catalysts. Most studies on platinum bimetallic catalysts have focused on changing the metals used, with not much attention on how the d-band theory affects the catalyst's performance. Herein, we investigated the additional of different transition metals alters the d-band center for better hydrogen evolution. A method combining the ultrasound processing and in-situ reduction was designed, resulting in the alloys with different stacking orders. As the d-band of transition metal elements in the alloy shifts upwards, the lower the energy of the alloy's d-band center, the better the stability of the adsorption bonding exhibited by the alloy. The PtCu/C, with a hexagonal-close-packed structure and a d-band center at −1.823 eV, has an 84 mV overpotential at 100 mA cm −2 , lower than PtNi/C (89 mV) and PtCo/C (91 mV). It also has 4.75 times the mass activity of commercial Pt/C. As a cathode catalyst, PtCu/C provides improved water-splitting at 2.31 V vs. 2.55 V for commercial Pt/C (at 1 A cm −2 ). This analytical strategy through the d-band center advances the design of platinum-based bimetallic catalysts and offers a new direction for the optimization and development of hydrogen evolution reaction electrocatalysts.
研究领域:
材料科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
·
IF 8.1
Fei Fan,Shiyu Han,Ying Li,Lu Qi,Jie Kang,Zhiping Chen,Chang Tian,DeChao Wang,Wenwu Zhou
The microenvironments including the surface hydroxyls , the oxygen vacancies , and the d-band center of hierarchical TS-1 zeolite pickled by hydrochloric acid were regulated by ZrO 2 , the effect of ZrO 2 on the physicochemical properties and the catalytic performances of the corresponding NiMoS supported catalysts were studied. The experimental and theoretical calculation results show that the d-band center, the surface hydroxyl groups , and the oxygen vacancies were regulated after incorporation of ZrO 2 . Resulting in the modulated acidity of the support and the metal support interaction of the catalysts, further promoting the formation of type-II NiMoS active phases. The catalytic performance evaluations show that catalyst NiMo/1-ZAT exhibits the superior HDS performance, kinetic study further demonstrated that the enhanced catalytic activity was mainly contributed by the improved direct desulfurization activity generated from the moderate support acidity, suitable MSI, highest sulfidation degrees, most type-II NiMoS active phase and highest activity of individual active sites.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Yong Yang,Jianfeng Jiang,Ya-Nan Feng,Zanyong Zhuang,Fei-Fei Chen,Dantong Zhang,Yan Yu
The strong CO 2 adsorption and facile CO desorption are a trade-off issue for CO 2 -to-CO photoreduction pathways. Synchronous optimization of these two steps remains a substantial hurdle and has been less explored. Herein, an O/N mixed coordinated Co-NTA (NTA: nitrilotriacetic acid), featuring an ultralong nanofiber architecture, is reported for efficient CO 2 photoreduction. The mixed coordination can regulate the positions of d -band center of Co sites and also d – p orbital coupling with coordination atoms, which are recognized as main activity descriptors. Consequently, free energies of both steps of CO 2 →*CO 2 and *CO→CO are well optimized, making the CO 2 -to-CO photoreduction pathways more favorable thermodynamically. By contrast, the classic N-coordinated Co-MeIm (MeIm: 2-methylimidazole) and O-coordinated Co-BDC (BDC: 1,4-benzenedicarboxylic acid) suffer from unfavorable CO 2 adsorption and intractable CO desorption, respectively. In addition, achiral NTA molecules can direct the growth of Co-NTA into one-dimensional (1D) nanofibers, while Co-BDC and Co-MeIm possess typical 2D nanosheet and 3D polyhedron architectures. The fast electron transport along the axis directions makes charge-transfer kinetics most efficient over 1D Co-NTA. The thermodynamic and kinetic benefits jointly contribute to the 1.8-fold increase in CO production over 1D Co-NTA.
研究领域:
材料科学
·
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Fang Li,Haili Lin,Huiqin Yu,Xuemei Jia,Shifu Chen,Jing Cao
Replacing the sluggish oxygen evolution reaction with the oxidation of benzyl alcohol to construct the hybrid water electrolysis system has been attractive for its merits of environmentally friendly and economically efficient. However, the activity of the catalyst to oxidize alcohols needs to be further improved. Tailoring the d-band center (E d ) has been proven as an effective method to promote the hydrogen evolution reaction (HER). How feasible is this strategy in the oxidation of benzyl alcohol? Here, using Co 2 C as a research platform, the doping nonmetal heteroatom (P, S, N) engineering is adopted to promote its electrocatalytic BA oxidation and HER performance. The results of electrochemical tests show that the P-doped Co 2 C (P–Co 2 C) only requires a low potential of 1.33 and 1.38 V vs. RHE to achieve current densities of 20 and 100 mA cm −2 for BA oxidation, which is superior to that of S–Co 2 C, N–Co 2 C, and pristine Co 2 C. The conversation and faradaic efficiency for BA is up to 98.1% and 93.8% during ten consecutive cycle tests. The P–Co 2 C also exhibited outstanding activity and stability toward HER. The density functional theory (DFT) calculation revealed that specified P doping could modify the d-band center of Co 2 C approaching the peak of the volcano map (electrochemical overpotentials ∼ E d ). The Gibbs free energy of the BA oxidation was also reduced, thus optimizing the adsorption and desorption process of intermediates. On the other hand, the catalyst surface physical properties of Co 2 C such as hydrophilicity was promoted by the doped heteroatoms which was favorable for the gas-liquid-solid triphase electrocatalytic reaction. This work offers a facial perception of regulating the d-band to design advanced bifunctional electrocatalysts for organic matter oxidation and HER.
研究领域:
电化学
·
材料科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）