ACS Catalysis
·
2023
·
IF 12.9
Xu Yu,Han Tian,Zhengqian Fu,Fenglai Pei,Lingxin Peng,Ge Meng,Fantao Kong,Yafeng Chen,Chang Chen,Ziwei Chang,Xiangzhi Cui,Jianlin Shi
The hydrogen spillover effect on metal-supported electrocatalysts is of great significance in hydrogen-involved reactions, especially in a hydrogen oxidation reaction (HOR). Herein, a facile thermal reduction method has been adopted to synthesize W18O49 (WO2.72) nanospheres decorated with single nickel atoms, and the obtained Ni-WO2.72-T (1.20 wt % Ni) was used as a probe catalyst for investigating the hydrogen spillover effect, which exhibits enhanced HOR performance, stability, and resistance to CO poisoning in acidic electrolytes. Based on in situ Raman spectroscopy and the density functional theory (DFT) calculation, a synergistic effect between Ni single-atom active sites and the hydrogen spillover effect is proposed to contribute to the HOR performance on Ni-WO2.72-T. Briefly, the introduction of single Ni atoms induces electron redistribution on Ni-WO2.72-T, making Ni atoms positively charged for H2 adsorption and activation, and on the other hand, the reversible phase transformation between WO2.72 and HxWO2.72 facilitates H* transfer from Ni to WO2.72, i.e., hydrogen spillover, resulting in elevating the HOR catalytic activity. Both experimentation and theoretical calculations demonstrate that the reversible phase transformation of the WO2.72 substrate strengthens the hydrogen spillover effect and thus elevates the HOR catalytic performance, which is believed to be helpful in designing highly active catalysts for hydrogen-involving reactions.
研究领域:
电化学
·
催化材料
·
理论计算
✓ 已验证
产品关联
DOI
高影响因子
Particuology
·
2024
·
IF 4.1
Jingchuan Wang,Junhong Luo,Yong Yao,Jiangfeng Song,Yan Shi
To improve room-temperature hydrogen storage, palladium (Pd) nanoparticles were innovatively decorated by carbon bridge onto the amino-group functioned Zr-terephthalate metal-organic framework (MOF) UiO-66 to reduce the diffusion energy barrier and then improve the hydrogen spillover effect. Powder X-ray diffraction shows broad Pd peak and retained UiO-66-NH 2 integrity after Pd decoration. The hydrogen uptake capacity show that UiO-66-NH 2 -Pd exhibits best hydrogen storage performance than UiO-66-NH 2 and pristine UiO-66. The hydrogen up taken in Pd decorated UiO-66 (UiO-66-NH 2 -1Pd) was close to 4 wt% under 20 MPa at room temperature. Density functional theory (DFT) calculations show that hydrogen adsorption energy of UiO-66-NH 2 -Pd was −0.5897 eV, which was much lower than that of UiO-66-NH 2 (−0.3716 eV) and UiO-66 (−0.2975 eV). Ultimately, Pd decorated NH 2 group functioned UiO-66 enable improve storage capacities through hydrogen spillover under ambient conditions which could satisfy the demand for sustainable energy, especially for the long-term storage energy media.
研究领域:
材料科学
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Lulu Zhang,Rui Li,Luyao Cui,Zijun Sun,Lijun Guo,Xiaochao Zhang,Yunfang Wang,Yawen Wang,Zhuobin Yu,Tao Lei,Xuan Jian,Xiaoming Gao,Caimei Fan,Jianxin Liu
Synergistic water activation and nitrogen reduction process is significant to the photocatalytic ammonia synthesis reaction, in which the obtainment of active hydrogen (H*) from H 2 O dissociation and then transfer to N 2 activation site is essential. Herein, the oxygen vacancies (OVs) enhanced hydrogen spillover is used to increase the H* transfer between the H 2 O activation site (Ru) and the N 2 activation site (OVs-rich W 18 O 49 ). Results shown that the OVs-rich Ru/W 18 O 49 achieves high activity for NH 3 production with a yield of 222.75 µmol‧g −1 ‧h −1 , which is 5.60 folds of the OVs-deficient Ru/W 18 O 49 . Control experiments, characterization, and theoretical calculation made it clear that OVs played crucial roles in enhancing the hydrogen spillover by modifying the support's Gibbs free energy for hydrogen adsorption and lowering the barrier of H* migration. Finally, the detail mechanism was explained from a new perspective. This strategy may provide new insights for other hydrogenation reactions under mild conditions.
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
FUEL
·
2024
·
IF 6.7
Zhaozhuo Yu,Wenzhuo Kong,Yaping Guo,Wen Liang,Jiawei Liang,Meijuan Chen,Dongxu Zhao,Hongzhen Ma,Xiangjun Liu,Solomon Inalegwu Okopi,Lei Che,Qi Zhang,Zhuohua Sun,Fuqing Xu
Eco-friendly lignin depolymerization into monomeric phenols in an aqueous system is essential for the sustainable and green valorization of lignocellulosic biomass. However, a major challenge in this process is the development of efficient and stable catalysts for aqueous reductive catalytic fractionation (RCF), as water can cause catalyst deactivation and reduce monomer yields. In this study, a water-resistant RuNiZnO x /Nb 2 O 5 catalyst is developed that demonstrates excellent catalytic activity and stability in aqueous systems, achieving a near-theoretical monomeric phenol yield of 40.1 wt% under reaction conditions of 240℃ and 3 MPa H 2 for 4 h. The excellent performance of this catalyst is attributed to the synergistic hydrogen spillover effect between Ni and Ru and the strong acidic properties of ZnO, as revealed by in-situ XPS analysis and NH 3 -TPD, respectively. This hydrogen spillover effect significantly alters the product composition, promoting the generation of POH-S/G from lignin model compounds. Additionally, screening of the catalyst support materials revealed that Nb 2 O 5 not only enhances Ru dispersion but also improves its stability, resulting in a minor decrease in lignin monomer yield observed after three cycles.
研究领域:
生物质化学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2025
·
IF 2.5
Yanfang Nie,Ye Tian,Ni Wang,Yunfan He,Yawen Wang,Yunfang Wang,Rui Li,Lulu Zhang,Jianxin Liu
An effective strategy for enhancing photocatalytic hydrogen evolution reaction (HER) activity is the implementation of the hydrogen spillover effect. Herein, a Ru/TiO2–GO (graphene oxide) catalyst was fabricated by means of simple hydrothermal and ultrasound-assisted techniques. By using the secondary hydrogen spillover process, which involves the transfer of active hydrogen species from Ru to TiO2 and then further to GO, the hydrogen evolution activity of Ru/TiO2–2GO reached 23.9 mmol g−1 h−1, which is 45.2 times and 3.85 times greater than that of TiO2 (0.53 mmol g−1 h−1) and Ru/TiO2 (6.2 mmol g−1 h−1), respectively. Controlled experiments and detailed characterization have revealed that the dispersion of GO on the support provides critical desorption sites for H*, thereby promoting the cleavage of Ti–H bonds. H* undergoes secondary spillover onto GO and desorbs to generate H2, enhancing the photocatalytic HER activity. This study enhances the photocatalytic activity of water splitting for hydrogen production by employing a secondary hydrogen spillover strategy, thereby presenting a novel approach for the design of efficient hydrogen production catalysts.
研究领域:
材料科学
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Fan Yang,Lulu Zhang,Feifei Li,Zhipeng Zhang,Luyao Cui,Rui Li,Caimei Fan,Jianxin Liu
Hydrogen spillover effects will significantly improve the activity of photocatalytic hydrogen evolution reactions (HER), while their introduction and optimization require the construction of an excellent metal/support structure. In this study, we have synthesized Ru/TiO 2-x catalysts with controlled oxygen vacancy (OVs) concentrations using a simple one-pot solvothermal method . The results show that Ru/TiO 2-x3 with the optimal OVs concentration exhibits an unprecedentedly high H 2 evolution rate of 13604 μmol·g −1 ·h −1 , which was 45.7 and 2.2 times higher than that of TiO 2-x (298 μmol·g −1 ·h −1 ) and Ru/TiO 2 (6081 μmol·g −1 ·h −1 ). Controlled experiments, detailed characterizations, and theoretical calculations have revealed that the introduction of OVs on the carrier contributes to the hydrogen spillover effect in the metal/support system photocatalyst and that the process of hydrogen spillover in this system can be optimized by modulating the OVs concentration. This study proposes a strategy to decrease the energy barrier of hydrogen spillover and enhance photocatalytic HER activity. Moreover, it investigates the effect of OVs concentration on the hydrogen spillover effect in the photocatalytic metal/supports system.
研究领域:
材料科学
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催化化学
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能源科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF CATALYSIS
·
2023
·
IF 7.3
Yujie Wan,Pengfei Ma,Hongliang Lu,Jianping Zhang,Jie Wang,Weiping Fang,Wenjing Song,Quanxing Zheng,Weikun Lai
Hydrogen spillover had played a significant role in catalytic processes involving reducible oxide supported metal catalyst and hydrogen molecule. Herein, crystal plane regulative hydrogen spillover strategy for the effective reductive amination on Ni/Al 2 O 3 was developed. A rod-like alumina supported Ni catalyst with primarily external (1 1 1) facets was prepared. In the presence of NH 3 and H 2 , Ni/Al 2 O 3 (1 1 1) exhibited a turnover number of 30.4 h −1 , which was 136-fold higher than that of Ni/Al 2 O 3 (1 1 0) in the reductive amination of furfural to furfuryl amine. For the Ni/Al 2 O 3 (1 1 1) catalyst, Al 2 O 3 (1 1 1) facets exhibited strong Lewis acidity, resulting in an enhanced H affinity of Al 2 O 3 (1 1 1) and a positively charged of Ni through electronic interaction. It was revealed that strong H affinity of Al 2 O 3 (1 1 1) and positively charged Ni sites significantly promoted hydrogen migration from Ni surface to Al 2 O 3 (1 1 1) facets, which effectively prevented the Ni sites from hydrogen poisoning and enhanced the adsorption and activation of NH 3 and intermediates for reductive amination. Consequently, the activation energy of Schiff base reductive ammonolysis was obviously reduced, resulting in high inherent activity for furfural reductive amination to furfuryl amine. This work developed a new strategy for high efficiency reductive amination catalyst in terms of hydrogen spillover effect.
研究领域:
催化化学
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材料科学
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能源化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2022
·
IF 10.53
Qinsheng Wang,Yiyi Fan,Chengliang Wu,Yun Jin,Claudia Li,Jaka Sunarso,Xiuxia Meng,Naitao Yang
Research on gas separation membrane has targeted upon maximizing the selectivity and permeance. The development of 2D materials ( e.g. , MXene) gives a novel avenue to surpass the “trade-off” among the membrane selectivity and permeability. However, randomly stacked nanosheets and the regulation of interlayer spacing for MXene nanosheets hinder the development of MXene membrane. To this end, we designed a Pd-intercalated lamellar MXene membrane to modify the surface chemical properties (H-spillover effect) of MXene (Ti 3 C 2 T x ) and to expand the interlayer spacing (from 2.29 to 3.26 Å) due to the strong interaction between Pd 2+ and MXene nanosheets with negative charge. Here, we performed a single-step etching approach to prepare 2D Pd-MXene membrane and demonstrated its excellent H 2 permeability of 2.66 × 10 −7 mol m −2 s −1 ·Pa −1 and H 2 /CO 2 selectivity of 242 at 25 °C, which greatly exceeds the current benchmark membranes. We also developed single gas transport mathematical mechanism models to interpret and support the experimental results. The combined experimental and modeling results show that interlayer spacing and H-spillover effect of Pd-MXene membrane benefit H 2 /CO 2 separation.
研究领域:
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
CERAMICS INTERNATIONAL
·
2025
·
IF 5.6
Bangqia Huang,Qingge Feng,Zequan Li,Qihua Liang,Guo-Dong Li
Given the potential hazards posed by triethylamine (TEA) to human health and environmental safety, it is crucial to have real-time and efficient detection methods in place. However, the low reactivity of TEA poses a challenge in achieving effective detection at low temperature. Hence, a high-performance sensor for detecting TEA was developed using Pd-doped WO 3 prepared through a one-step electrospinning method. The sensor based on 1.0 wt% Pd-WO 3 exhibited exceptional performance in detecting TEA at low temperature (100 °C), showing a response of 246 to 20 ppm. Additionally, it demonstrated a low detection limit (0.03 ppm) and excellent selectivity characteristics. The outstanding sensing capability can be ascribed to the noble metal electron sensitization and spillover effects, which enhance the interaction between chemisorbed oxygen and TEA gas by adjusting the Fermi level of 1.0 wt% Pd-WO 3 . This adjustment achieves surface electron redistribution and optimizes interfacial atomic transport, while also reducing the activation energy required for gas sensing, thereby lowering the operating temperature.
研究领域:
材料科学
·
环境科学
·
传感器技术
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Jiayu Jin,Shuozhen Hu,Xinsheng Zhang,Shigang Sun
Palladium is a promising formic acid electro-oxidation (FAO) catalyst due to its higher initial activity than platinum. However, suffering from the adsorption of hydrogen and CO-like species, the activity and stability of Pd are still unsatisfied. Herein, palladium nanoparticles deposited on carbon supported molybdenum trioxide (Pd–MoO 3 /C) is prepared with MoO 3 as the promoter for FAO. X-ray photoelectron spectroscopy analysis proves the close contact between Pd and MoO 3 , which generates the hydrogen spillover effect and forms the Pd–Mo structure. The hydrogen spillover effect enhances the desorption of hydrogen from Pd and facilitates the FAO activity. Both the spillover effect and Pd–Mo structure contribute to the removal of CO ad and facilitate the durability and anti-CO poisoning ability of the catalyst. With the optimized ratio of MoO 3 to carbon black, the Pd–MoO 3 /C-20 catalyst owns the best specific activity of 5.86 mA cm −2 , which is 1.86 times of Pd/C.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 13
·4200-4206
·
IF 4
Jianxin Lv,Linghui Zhang,Lianxi Si,Hui Li,Wenbo Zhao,Fei An,Xia Feng,Shi Hu
Materials with accurate and durable gas detection are essential for gas sensors. We developed a facile and effective method to deposit Pd onto WO3 nanosheets and used the samples for hydrogen gas sensing. The combination of the 2D ultrathin nanostructure of WO3 and the spillover effect of Pd enables a detection concentration down to 20 ppm of hydrogen and high selectivity against other gases including methane, butane, acetone, isopropanol, etc. Moreover, the durability of the sensing materials was testified through 50 cycles of exposure to 200 ppm of hydrogen. These outstanding performances are mainly attributed to a homogeneous and tenacious decoration of Pd on the surface of WO3 nanosheets, providing an attractive choice for practical applications.
研究领域:
材料科学
·
纳米技术
·
气体传感
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Hongyu Wang,Kai Zhang,Lanlan Wu,Yanji Wang,Xiaohang Du,Jingde Li
The development of active and durable low-Pt electrocatalysts for oxygen reduction reaction (ORR) is the key target for proton exchange membrane fuel cells. Herein, a charge transfer and spillover effect enabled efficient ordered porous titanium dioxide supported PtCu alloy-based carbon-free ORR catalyst (PtCu@TiO 2-x N) is developed. Experimental characterization and theoretical analysis reveal that the rich oxygen vacancies and N-doping of TiO 2 support promotes the electron transfer from PtCu to TiO 2-x N, resulting in electron-deficient PtCu surface. This weakens the adsorption of ORR intermediates on PtCu, and simultaneously promotes their spillover from PtCu sites to adjacent TiO 2-x N support. This dynamic renewal of the PtCu active sites allows the rapid proceed of ORR, and thus accelerating its reaction kinetics. Accordingly, the PtCu@TiO 2-x N catalyst exhibits greatly enhanced ORR activity with a specific activity of 1.83 mA cm −2 Pt , mass activity of 1.24 A mg −1 Pt and excellent durability as well. The results show that the rational design of Pt-based catalyst with spillover effect is of great significance towards efficient ORR reaction.
研究领域:
材料科学
·
电化学
·
催化作用
✓ 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）