Catalysis Science & Technology
·
2024
·Vol. 14
·期 10
·2825-2837
·
IF 4.4
Bin Kang,Mengfei Guo,Haotian Wu,Xiaonan Guo,Zhaoying Di,Ying Wei,Jingbo Jia,Zhou-jun Wang,Runduo Zhang
In this study, a series of alkali/alkaline-earth-metal doped Co3O4 spinel oxides was prepared for N2O catalytic decomposition. It was found that doping with alkali/alkaline-earth-metal ions essentially caused lattice distortion of M–Co3O4, decreased the crystal size, and increased the specific surface area and Co2+ (active sites) amounts. Physicochemical characterization of these as-prepared catalysts was performed, including Raman, XPS, H2-TPR, O2-TPD, and OIE, to indicate that M–Co3O4 has a high lattice oxygen mobility and is prone to form more oxygen vacancies. These oxygen vacancies were involved in N2O decomposition and synergistically promoted the reaction cycle of Co2+ sites. The catalytic activities were ranked in the order of Co3O4 < Mg–Co3O4 < Na–Co3O4 < Ca–Co3O4 < K–Co3O4 < Rb–Co3O4 < Cs–Co3O4, among which the best-performing sample (Cs–Co3O4) had a T90 that was nearly 200 °C lower than that of pure Co3O4, with the complete conversion of N2O achieved at 350 °C. In addition, the effects of alkali/alkaline-earth-metal doping on the lattice distortion, oxygen vacancy formation, N2O dissociation, and oxygen recombination and desorption of M–Co3O4 were verified using DFT calculations.
研究领域:
催化化学
·
环境化学
·
材料科学
·
物理化学
·
无机化学
✓ 已验证
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2021
·
IF 3.764
Liqi Xiao,Zean Xie,Shaojia Song,Zhiping Zhao,Ming Ke,Weiyu Song,Zhen Zhao,Jian Liu
Recently, coordinated unsaturated TiO2 due to the oxygen vacancy has been found to have good application prospects in propane dehydrogenation (PDH) reactions. The oxygen vacancy can be effectively adjusted by metal doping into TiO2. In the present paper, density functional theory calculations were conducted to study the PDH reaction of TiO2 doped with transition metals in the fourth period with the aim to screen for an effective doping metal. A good linear relationship was found between the calculated turnover frequency and co-adsorption energy of H and Propyl species, justifying such co-adsorption energy as a useful descriptor for screening PDH catalysts. Compared with pure-phase TiO2, V-doped TiO2 exhibits a lower propane C–H bond breaking energy barrier (0.93 eV) and a higher TOF (5.67 × 10–3 s–1) value. According to the calculation results, the V-doped TiO2 catalyst was successfully synthesized. The experimental results show that the r(C3H6) rises with V doping.
研究领域:
材料科学
·
化学工程
·
催化反应
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Xiaomei Xu,Bilu Yang,Zhaodi Xu,Qiaoling Mo,Xiaomei Shen,Hu Cai
In the pursuit of advancing the production of H 2 through hydrogen-evolution reaction (HER), the demand for the elaborate design of cost-effective and robust durability electrocatalysts has gained momentum, especially replacement of noble-metal counterparts like Pt. Herein, we introduce a facile one-pot hydrothermal approach to synthesize nickel foam-supported Ni 3 S 2 nanosheet arrays, which integrate with carbon-quantum-dot (CQDs) and Cu, Mo dual-metal doped. With the introduction of CQDs and Cu, Mo dual-metal doped site, the optimal CQDs-Cu-Mo-Ni 3 S 2 @NF exhibits superior HER catalytic activity with a low overpotential of 125 mV at 10 mA·cm −2 and strong durability for 30 h in alkaline medium. The exceptional electrocatalytic performance is ascribed to the synergistic effect of CQDs and Cu, Mo dual-metal site. This synergy encompasses optimization of water molecule adsorption/desorption energetics , elevated electrical conductivity , weakening of the strong S–H bond interaction on the Ni 3 S 2 surface, and providing ample active centers. Furthermore, an in-depth understanding of the electronic structure and adsorption energy during the HER process is probed by density functional theory (DFT) analysis. Our work provides a quintessential paradigm for the rational design of multi-component electrocatalysts for water splitting.
研究领域:
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
MOLECULES
·
2025
·Vol. 30
·期 11
·2343
·
IF 4.6
Xinyue Li,Yahui Song,Yiming Huang,Jihui Zhang,Siyu Wu,Wentao Zhang,Jin Wang,Xian Zhang
MoS2has emerged as a highly promising catalyst for the hydrogen evolution reaction (HER) owing to its exceptional catalytic properties. However, there is a pressing need to further enhance its reactivity and integrate oxygen evolution reaction (OER) capabilities to facilitate its industrial implementation. In this context, a dual-metal doping approach presents a straightforward and effective strategy to achieve superior catalytic performance. Systematic characterization and electrochemical evaluations reveal that the synergistic effects of Co and Fe doping significantly enhance both HER and OER activities, demonstrating remarkable potential for practical applications in energy conversion and storage systems. The unique flower-like architecture of the material endows it with a substantially enlarged surface area, which significantly increases the exposure of active sites and facilitates enhanced catalytic activity. Specifically, it achieves the low overpotentials of −127 and 292 mV at 10 mA cm−2for HER and OER in alkaline media, respectively, and demonstrates excellent stability over a 10 h test. This research provides valuable insights into the development of advanced materials capable of efficiently performing both HER and OER processes, paving the way for potential applications in sustainable energy technologies.
研究领域:
材料科学
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电催化
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能源转换与存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2025
·
IF 9.5
Qiang Fu,Zhiling Huang,Zheming Ni,Shengjie Xia
Effectively enhancing nitrogen activation and inhibiting water splitting reactions are key factors in photocatalytic nitrogen reduction. This work integrated defect engineering and metal doping, doping transition metals Sc, Cu, and V into molybdenum sulfide (MoS2) containing sulfur vacancies (VS) to prepare TM@VS−MoS2(TM=Sc, Cu, V), applied for photocatalytic nitrogen reduction (pNRR). High angle annular dark field scanning transmission electron microscopy (HAADF-STEM) confirms the existence of S vacancies. The pNRR activity of Sc@VS−MoS2, Cu@VS−MoS2 and V@VS−MoS2 is 124.26 μmol g−1 h−1, 101.32 μmol g−1 h−1, 88.64 μmol g−1 h−1, respectively, which is much higher than that of MoS2, VS−MoS2, and TM@MoS2. This fully demonstrates that the comprehensive use of S vacancies and metal doping can significantly enhance the photocatalytic performance of MoS2 (with a maximum activity improvement of nearly 5 times). DFT calculations show that transition metal doping can further promote the activation of N2 and inhibit the production of H2 from water decomposition for vacancy MoS2. The effect of the above promotion and inhibition is consistent with the order of activity and photoelectronic properties: Sc@VS−MoS2>Cu@VS−MoS2>V@VS−MoS2. In situ infrared spectroscopy revealed the generation of −N2Hy (1≤y≤4) active species during the pNRR process, which is consistent with the most potential pathway (enzymatic mechanism) calculated by DFT.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL PHYSICS LETTERS
·
2020
·
IF 2.029
Hao Zhang,Yunqing Tang,Zhixiang Liu,Zhi Zhu,Xu Tang,Yemei Wang
Alkali metal (Li, Na, K and Rb) doped g-C 3 N 4 were prepared by water bath heating and high temperature calcination method. Photoelectric properties were studied by first-principles calculations and experiments. Computational results show that absorption spectra of Rb doped g-C 3 N 4 increases significantly in the wavelength range of 500–1100 nm, which is consistent with the UV–vis spectrum. Rb doped g-C 3 N 4 showed the best photo-reduction CO 2 performance, with a CO productivity more than three times higher compared with bulk g-C 3 N 4 . This work provides a guiding significance for construction of doped g-C 3 N 4 materials applied in fields of environmental remediation, energy conversion and medical imaging.
研究领域:
材料科学
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环境科学
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能源科学
✓ 已验证
产品关联
DOI
高影响因子
ChemSusChem
·
2023
·Vol. 16
·期 8
·e202202257
·
IF 8.4
Wensheng Yang,Xinhai Wang,Shengshang Lu,Yue Gao,Tinghong Gao,Tong Guo,Quan Xie,Yunjun Ruan
Graphical Going uphill : The dissolution mechanism of sodium vanadium phosphate (NVP) in an aqueous electrolyte is investigated in detail. Using metal (Fe or W) doping can enhance the strength of the metal-oxygen bond to suppress partial vanadium dissolution in NVP. Furthermore, the synergy of bimetallic doping completely inhibits V dissolution to improve the cycling stability of NVP. Aqueous sodium-ion batteries (ASIB) offer many potential applications in large-scale power grids since they are inexpensive, safe, and environmentally friendly. Sodium superionic conductors (NASICON), especially carbon-coated Na 3 V 2 (PO 4 ) 3 (NVP), have attracted much attention due to the full use of their high ion migration speed. However, the poor cycle lifespan and capacity retention of NVP hinder its application in ASIB. Herein, a novel bimetal-doped Na 3 V 1.3 Fe 0.5 W 0.2 (PO 4 ) 3 (NV 1.3 Fe 0.5 W 0.2 P) cathode is designed and synthesized to achieve outstanding cycling stability (95 % of initial capacity at 50th cycle). The electrochemical behavior and charge storage mechanism of NV 1.3 Fe 0.5 W 0.2 P are systematically investigated by various in situ and ex situ characterizations. The Fe and W codoping could stabilize the NASICON framework to suppress the proton attack on the Na site in the aqueous electrolyte, thus resulting in excellent cycling stability. DFT calculations show that bimetallic doping increases the structural stability of NVP. Moreover, an ASIB fabricated using a NV 1.3 Fe 0.5 W 0.2 P cathode and a NaTi 2 (PO 4 ) 3 anode delivers 64 mAh g −1 at room temperature, 95 % capacity retention after 50 cycles (1 A g −1 ).
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2023
·
IF 16.5
Ning Zhang,Jiayi Du,Na Zhou,Depeng Wang,Di Bao,Haixia Zhong,Xinbo Zhang
Proton-exchange membrane water electrolysis, particularly driven by renewable electricity, is a sustainable strategy for green hydrogen production . However, developing highly active and stable electrocatalysts to accelerate the oxygen evolution reaction (OER) remains challenging. Herein, we introduce an effective strategy for constructing high-valence metal-doped IrO x with abundant oxygen vacancies, while simultaneously enhancing the catalytic activity and stability of the acidic OER. The synthesized Ta-doped IrO x (350-Ta@IrO x ) exhibits ultramicroscopic nanoparticle morphology and abundant surface oxygen vacancies, enabling a rapid OER process with a low overpotential of 223 mV at 10 mA cm -2 and 147.7 times higher mass activity (1207.4 A g Ir −1 ) than that of commercial IrO 2 at 1.55 V versus the reversible hydrogen electrode. More importantly, 350-Ta@IrO x affords excellent stability with insignificant potential degradation after 500 h of electrolysis at 10 mA cm 2 , originating from the low operating potential and suppressed dissolution and oxidation of oxygen vacancy active sites via Ta doping. Density functional theory calculations suggest that Ta doping and oxygen defect engineering are effective in facilitating the nucleophilic attack of water molecules, thereby accelerating the rate-determining step toward high catalytic OER activity on Ta-doped IrO x . We anticipate that this study will provide an effective method to obtain active and stable electrocatalysts via high-valence metal doping.
研究领域:
化学
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材料科学
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能源科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2023
·
IF 4.5
Xiaoxi Li,Jiajia Li,Dilnur Kurbanjan,Tianhao Yu,Hong Du
Zeolite imidazole frameworks (ZIFs) structures are widely used as an efficient catalyst for metal organic frameworks (MOFs) in electrocatalysis. In this work, the structure of the trimetallic ZIFs sample was rationally designed by the method of doping with Ni 2+ and Zn 2+ . After that, a layer of highly conductive π-π conjugated organic molecules was wrapped on the trimetallic ZIFs sample to form a heterojunction structure of NiZnCo-ZIF@HHTP composite. The activity of oxygen evolution reaction (OER) of NiZnCo-ZIF was improved after it was combined with HHTP. NiZnCo-ZIF@HHTP presents a low overpotential (η ≈ 193 mV @10 mA cm −2 ), a small Tafel slope (97.4 mV dec −1 ) and outstanding stability for OER in 1 M KOH solution. The superior OER performance of NiZnCo-ZIF@HHTP is due to the effect of doping of Ni and Zn to form a trimetallic ZIF material. The synergistic effect of Ni Zn codoped enhances the conductivity of ZIF-67 material. Meanwhile, the π-π conjugation effect of HHTP organic macromolecule can further enhance the electrical conductivity of NiZnCo-ZIF. The result suggests that the co-doping of polymetallic cations and the coating of conducting organic molecules can be vital for modifying ZIFs electrocatalysts. This work provides a meaningful reference value for modifying non-precious metal ZIFs materials in electrocatalysis.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
·
2021
·Vol. 96
·期 8
·2238-2248
·
IF 3.174
Xiao-Yang Yue,Hui-Fang Ren,Chengming Wu,Jun Xu,Jifan Li,Chun-Ling Liu,Wen-Sheng Dong
BACKGROUND Methyl lactate is widely applied in the chemical, food, cosmetics and pharmaceutical industries. The conversion of carbohydrates over heterogeneous catalysts to methyl lactate is a promising environmentally benign process. RESULTS Hierarchical Sn-Beta zeolite (Sn-Beta) and corresponding bimetal-doped Beta zeolites (M-Sn-Beta; M = Zn, In, La, Ga, Ni) were prepared via a novel modified hydrothermal synthesis method to convert carbohydrates into methyl lactate. The introduction of Zn into Sn-Beta considerably improved the yield of methyl lactate from glucose, while for the catalysts containing In, La, Ga and Ni, such improvements were not observed. CONCLUSIONS A methyl lactate yield reaching up to 66.7% was obtained over Zn-Sn-Beta at 220 °C for 6 h. The enhanced catalytic performance was attributed to high Lewis acid density and strength, together with synergistic effects between framework Sn 4+ and Zn 2+ ions of Zn-Sn-Beta. Additionally, Zn-Sn-Beta demonstrated fructose and sucrose conversion into methyl lactate with yields of 68.4% and 70.0%, respectively. The Zn-Sn-Beta catalyst could be re-used at least five times with only a slight loss of methyl lactate yield. © 2021 Society of Chemical Industry (SCI).
研究领域:
化学工程
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Jing Chen,Mingzheng Gu,Shoujie Liu,Tian Sheng,Xiaojun Zhang
Modifying the electronic structure of electrocatalysts by metal doping is favorable to their electrocatalytic activity. Herein, by a facile one-pot redox process of Fe(III) and Cu(I), Fe(II) was successfully doped into the subsurface of CuS nanosheets (NSs) for the first time to obtain a novel electrocatalyst (Fesub-CuS NSs) that possesses not only subtle lattice defects but also an atomic-level coupled nanointerface, greatly enhancing the oxygen evolution reaction (OER) performances. Meanwhile, Fe(II) and Fe(III) coexisting in Fesub-CuS nanosheets are favorable to OER through valence regulation. As expected, by simultaneously controlling the abovementioned three factors to optimize Fesub-CuS nanosheets, they display a lower overpotential of 252 mV at a current density of 20 mA cm–2 for OER, better than 389 mV for pristine CuS nanosheets. This discovery furnishes low-cost and efficient Cu-based electrocatalysts by metal doping. Density functional theory (DFT) calculations further verify that Fesub-CuS(100) is thermodynamically stable and is more active for OER. This research provides a strategy for the atomic-scale engineering of nanocatalysts and also sheds light on the design of novel and efficient electrocatalysts.
研究领域:
材料科学
·
电催化
✓ 已验证
产品关联
DOI
PubMed
高影响因子
TRANSACTIONS OF NONFERROUS METALS SOCIETY OF CHINA
·
2018
·
IF 1.795
Qiu-hang CHEN,Shi-liang MEI,Wu YANG,Wan-lu ZHANG,Gui-lin ZHANG,Jia-tao ZHU,Rui-qian GUO
Color tunable quantum dots (QDs) based on the Cu, Mn, Ag co-doped ZnInS core and ZnS outer-shell were synthesized by using an eco-friendly method. Core-shell doped QDs with the average size of 3.85 nm were obtained by using a one-pot synthesis followed by a hot injection with n -dodecanethiol (DDT) and oleylamine (OLA) as stabilizers in oil phase. Cu, Mn and Ag ions were introduced as single-dopant or co-dopants during the synthesis, providing an effective means to control the emission color of the QDs. The as-synthesized QDs showed photoluminescence emission ranging from green (530 nm) to near-red (613 nm), adjusted by doping components, dopant concentration, and Zn/In ratio. Importantly, quasi-white emission has been achieved by controlling the concentration of co-doped metal ions (Mn, Cu and Ag). The primary results demonstrated the promising potential of co-doped QDs as alternative materials for future high quality white LED applications.
研究领域:
材料科学
·
纳米技术
✓ 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）