APPLIED CATALYSIS A-GENERAL
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2025
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IF 4.8
Zhenwen Yang,Ziyi Shui,Ben Niu,Xiaoxiao Duan,Zheng Wei,Guoxia Jiang,Zhengping Hao
NH 3 decomposition is receiving increased attention for on-site CO x -free H 2 generation. Unfortunately, the harsh reaction conditions often cause sintering of active metals. Here we report a simple method to achieve well Ni dispersion by nano-structuring the BN support with La species. The surface reaction-induced LaBO 3 nano-islands on BN support have a strong affinity for Ni atoms, which can capture and confine Ni species to yield a large population of well dispersed Ni clusters and nanoparticles. The Ni species selectively anchored on LaBO 3 islands expose more active sites and boost desorption of N 2 and H 2 , exhibiting superior activity and stability for NH 3 decomposition. In addition, it is revealed that the Ni dispersion is sensitive to the change of the support surface structure. These findings highlight the important role of support structure in determining the nature of the metal phase and provide guidance for designing catalysts with controlled catalytic structure and reactivity.
研究领域:
催化化学
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材料科学
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产品关联
DOI
高影响因子
Biointerphases
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2019
·Vol. 14
·期 6
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IF 2.009
Cheng Fang,Ma Xiaochun,Feng Qiancheng,Wang Hanqi,Yin Meng,He Wei
The reliability and stability of array slides are a big concern for array vendors and end users. Herein, we report on a new type of array slide with high reactivity toward DNA probes and low side reaction. A one-step surface reaction via the Michael addition involved in preparing array slides was developed and characterized by x-ray photoelectron spectroscopy, contact angle, and fluorescence labeling. The effects of array fabrication and storage conditions, i.e., spotting solution p H, high humidity, and long-term storage on the reactivity of the slides were examined. The fabricated DNA arrays could realize good hybridization efficiency (38.2% for slides with 0.88 pmol/cm 2 ), low limit of detection (4 × 10 −14 M), as well as high mismatch selectivity.
研究领域:
分子生物学
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生物化学
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DOI
PubMed
高影响因子
Surfaces and Interfaces
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2024
·
IF 5.7
Xinyu Jiang,Fengtong Ju,Zhe Wu,Qiuyu Jing,Wenjing Lv,Yongchao Lai,Xiaomei Li
As a molecular-specific and highly sensitive technology, surface-enhanced Raman spectroscopy (SERS) is well-suited to meet the analytical demands of a multidisciplinary range of fields. Nevertheless, the fabrication of SERS substrates that are inexpensive, reproducible, and controllable represents a significant challenge. In this study, a straightforward, reproducible, and controllable strategy was proposed for the fabrication of high-sensitivity SERS substrates based on self-limiting surface reactions. The preparation of the self-confined nanogaps (sCN-Ag) substrate was achieved through the dealloying process of Cu-Ag alloy wires. In this process, the interior nanogaps were self-confined by AgCl produced in situ, thus facilitating the control of "hot spots" on a nanoscale. The sCN-Ag substrate, which can be readily activated by the removal of AgCl with NH₃·H₂O, exhibited high sensitivity, spatial uniformity, and good thermal stability in pH sensing. This self-limiting strategy, which integrates the advantages of controllability, reproducibility, and mass production, is expected to further promote the development and application of SERS.
研究领域:
分析化学
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材料科学
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纳米技术
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DOI
高影响因子
CATALYSIS TODAY
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2022
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IF 6.562
Li Tan,Yanru Li,Qian Lv,Yuyan Gan,Yuan Fang,Yu Tang,Lizhi Wu,Yuanxing Fang
The conversion of CO 2 to valuable chemicals by photocatalysis has attracted widespread interesting. Owing to the linear structure of CO 2 molecule with strong C O bond, the surface reaction is considered as one of the main issues to restrict the conversion efficiency. Herein, soluble UiO-66 has been developed as co-catalyst to enhance the photocatalytic performance for CO 2 reduction. The soluble UiO-66 has presented the performance ca. 1.5 higher than the insoluble version, yielding 30.6 µmol/h for CO 2 to CO conversion by using 5.0 mg sample. This improvement can be attributed to the preserved framework by soluble UiO-66. Therefore, the chemisorption of CO 2 molecules can be improved, boosting the reduction reaction for CO production. This research provides a new path for a rational design of metal-organic framework (MOF) for photoredox catalysis, meanwhile inspiring advanced application of MOF catalysis with the soluble manner.
研究领域:
化学
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材料科学
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环境科学
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产品关联
DOI
高影响因子
Journal of the American Chemical Society
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2022
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IF 16.383
Hongyu Chen,Pan Gao,Zhengmao Liu,Lixin Liang,Qiao Han,Zhili Wang,Kuizhi Chen,Zhenchao Zhao,Meiling Guo,Xuebin Liu,Xiuwen Han,Xinhe Bao,Guangjin Hou
Surface metal hydrides (M–H) are ubiquitous in heterogeneous catalytic reactions, while the detailed characterizations are frequently hindered by their high reactivity/low concentration, and the complicated surface structures of the host solids, especially in terms of practical solid catalysts. Herein, combining instant quenching capture and advanced solid-state NMR methodology, we report the first direct and unambiguous NMR evidence on the highly reactive surface gallium hydrides (Ga–H) over a practical Ga2O3 catalyst during direct H2 activation. The spectroscopic effects of 69Ga and 71Ga isotopes on the 1H NMR signal are clearly differentiated and clarified, allowing a concrete discrimination of the Ga–H signal from the hydroxyl crowd. Accompanied with quantitative and two-dimensional NMR spectroscopical methods, as well as density functional theory calculations, information on the site specification, structural configuration, and formation mechanism of the Ga–H species has been revealed, along with the H2 dissociation mechanism. More importantly, the successful spectroscopic identification and isolation of the surface Ga–H allow us to clearly reveal the critical but ubiquitous intermediate role of this species in catalytic reactions, such as propane dehydrogenation and CO2 hydrogenation reactions. The analytic approach presented in this work can be extended to other M–H analysis, and the insights will benefit the design of more efficient Ga-based catalysts.
研究领域:
催化化学
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材料科学
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物理化学
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产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Peiyang Gu,Feiyang Tan,Wuzi Zhao,Jingwen Dong,Shiyuan Zhou,Xiaoqiong Hao,Shengsheng Gu,Guangfeng Liu,Danfeng Wang
Photocatalysis has unprecedently prevailed in the removal of pollutants and the artificial photosynthesis of H 2 O 2. However, inefficient surface reaction and exciton dissociation rate are the main hurdles in arriving at high photocatalytic performance. A versatile strategy for improving surface reactions between the photocatalyst and the reactant and the charge separation dynamics is in pressing need. Herein, post-quaternization of the conjugated microporous polymer (CMP) is proposed. This not only converts the CMP from hydrophobic to hydrophilic but also evidently improves charge separation and mobility due to the polarizing effect. Most importantly, because of the quaternization, the surface reactions can be pronouncedly strengthened due to both the improved dispersity and lowering of O 2 adsorption energy. As a result, the CMPs serve both photodegradation and photosynthesis of H 2 O 2 , with iB-TDZ exhibiting pronounced enhancement in the photodegradation of 100 ppm of Congo red and 2,4-D in 40 min and 90 min, respectively, transcending the vast majority of the reported photocatalysts, while the production of H 2 O 2 reaches 2.922 mmol g −1 in three-hour irradiation. As a proof-of-concept experiment, simultaneous photodegradation of 2,4-D and photocatalytic H 2 O 2 production is realized. It was found that 2,4-D can boost photocatalytic H 2 O 2 production from 1.92 mmol g −1 (without 2,4-D) to 3.25 mmol g −1 within 90 min, likely due to its role in providing protons and serving as an h + scavenger. These findings provide a fresh platform for the design of CMP-based photocatalysts for simultaneous photocatalytic wastewater treatment and H 2 O 2 production.
研究领域:
环境科学
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材料科学
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催化化学
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产品关联
DOI
高影响因子
Journal of the American Chemical Society
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2021
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IF 15.419
Qing-Xia Chen,Ying-Huan Liu,Zhen He,Jin-Long Wang,Jian-Wei Liu,Hui-Jun Jiang,Wei-Ran Huang,Guan-Yin Gao,Zhong-Huai Hou,Shu-Hong Yu
The kinetics of electrode reactions including mass transfer and surface reaction is essential in electrocatalysis, as it strongly determines the apparent reaction rates, especially on nanostructured electrocatalysts. However, important challenges still remain in optimizing the kinetics of given catalysts with suitable constituents, morphology, and crystalline design to maximize the electrocatalytic performances. We propose a comprehensive kinetic model coupling mass transfer and surface reaction on the nanocatalyst-modified electrode surface to explore and shed light on the kinetic optimization in electrocatalysis. Moreover, a theory-guided microchemical engineering (MCE) strategy has been demonstrated to rationally redesign the catalysts with optimized kinetics. Experimental measurements for methanol oxidation reaction in a 3D ordered channel with tunable channel sizes confirm the calculation prediction. Under the optimized channel size, mass transfer and surface reaction in the channeled microreactor are both well regulated. This MCE strategy will bring about a significant leap forward in structured catalyst design and kinetic modulation.
研究领域:
化学工程
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电化学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF MEMBRANE SCIENCE
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2021
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IF 8.742
Peng Zhang,Song Wang,Bingjie Pang,Xuefeng Zhu,Weishen Yang
High temperature dual-phase mixed conductor membranes are promising for CO 2 separation and utilization. Most efforts are focused on materials, thickness, microstructural features and surface modifications of the electronic conducting phase. Here, we unveil the effect of the carbonate-ionic conducting phase on CO 2 permeation process with a dense NiO-based dual-phase membrane. The results demonstrate that the CO 2 flux increases first and then decreases with the increase of Li 2 CO 3 addition amount. The controlling step of CO 2 permeation changes from bulk diffusion to surface reaction as much more Li 2 CO 3 was added into the carbonate-ionic conducting phase. Model analysis indicates that the peroxide formation process on the membrane surface is the rate-limiting step, which is closely related to the oxygen solubility of molten carbonate.
研究领域:
材料科学
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化学工程
✓ 已验证
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2022
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IF 11.357
Hongchao Li,Na Yuan,Jieshu Qian,Bingcai Pan
The environmentally benign Mn oxides play a crucial role in the transformation of organic contaminants, either through catalytically decomposing oxidants, e.g., peroxymonosulfate (PMS), or through directly oxidizing the target pollutants. Because of their dual roles and the complex surface chemical reactions, the mechanism involved in Mn oxide-catalyzed PMS activation processes remains obscure. Here, we clearly elucidate the mechanism involved in the Mn2O3 catalyzed PMS activation process by means of separating the PMS activation and the pollutant oxidation process. Mn2O3 acts as a shuttle that mediates the electron transfer from organic substrates to PMS, accompanied by the redox cycle of surface Mn(IV)/Mn(III). Multiple experimental results indicate that PMS is bound to the surface of Mn2O3 to form an inner-sphere complex, which then decomposes to form long-lived surface reactive Mn(IV) species, without the generation of sulfate radicals (SO4•–) and hydroxyl radicals (HO•). The surface reactive Mn(IV) species are proposed to be responsible for the degradation of organic contaminants (e.g., phenol) and the formation of singlet oxygen (1O2), followed by the regeneration of the surface Mn(III) sites on Mn2O3. This study advances the fundamental understanding of the underlying mechanism involved in transition metal oxide-catalyzed PMS activation processes.
研究领域:
环境科学
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催化化学
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DOI
高影响因子
Surfaces and Interfaces
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2021
·
IF 4.837
Fan Wu,Chuan Pu,Minxian Zhang,Bin Liu,Jingling Yang
Solar photocatalysis is a clean and sustainable approach for removing atmospheric NO, but suffers from unsatisfactory removal efficiency. Efficient charge separation and surface reaction are critical factors ensuring the efficiency of solar energy conversion by photocatalysts. To achieve efficient charge steering and an enhanced surface reaction, we synthesized a bicomponent photocatalyst consisting of multivalent Ag species embedded in defect-rich twin-brush ZnO (Ag/TB-ZnO) with strong metal-support interaction (SMSI). The optimum Ag/TB-ZnO with silver loading of 2.0 wt.% achieved NO oxidation efficiency of 71.0% under a GHSV of 1,200,000 mL h −1 g −1 , and NO 3 − selectivity of 94.8%. Outstanding stability of up to 4 h was demonstrated. This superior performance was attributed to the enhanced efficacy of charge separation and surface reaction by the SMSI effect, surface plasmon resonance effect of metallic Ag and the efficient activation of oxygen species through vacancy-rich TB-ZnO.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
FUEL
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2022
·
IF 8.035
Chaohe Zheng,Mingze Su,Haibo Zhao
As the kinetic influencing factors were not considered properly in the previous studies, the obtained activation energies of copper oxidation were discrepantly ranging from 15.0 kJ/mol to 100.0 kJ/mol. The gas diffusion in the crucible and sample layer, the surface reaction and the defect diffusion of copper cations all have an impact on the conversion process of copper oxidation samples. Using the high diameter-height ratio crucible in our self-made TGA could effectively eliminate the gas diffusion in the crucible and reduce the error of the kinetic tests. Based on the previous four-step oxidation mechanism, the kinetic parameters of copper oxidation are identified using a grain-scale kinetic model, coupling with a defect transport model. The potential kinetic impact factors including the particle polydispersity, gas diffusion, defect diffusion, surface reaction and particle sintering are adequately considered in this work. First, it is found that the copper oxidation is not dominated by the defect diffusion in the solid product layer, but governed by the surface reaction in the gas–solid interface. The copper oxidation is likely to be adsorption-limited during the surface reaction in the gas–solid interface, and the intrinsic activation energy is identified as 48.0 kJ/mol. The particle-scale model is then performed to investigate the impact of physical properties of oxygen carrier particles. It can significantly accelerate the conversion rate of copper oxidation by means of decreasing the particle size and increasing the porosity. However, it is not advisable to decrease the grain size too much when preparing the oxygen carriers, for this will only increase diffusion resistance inside the particle for small grain. Finally, it can be found that in most conditions of the air reactor, Cu-based oxygen carrier with the grain size of 220–300 nm exhibits the best oxidation performance.
研究领域:
化学工程
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能源科学
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产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Tianyue Wang,Jia Liu,Bining Tian,Lulu Yan,Zhanfeng Li,Yue Tian
Engineering surface reaction kinetics plays a vital role in promoting CO2 photoreduction reaction (CO2 PRR) efficiency but remains formidably challenging. Here, we demonstrate that the regulation of the surface oxidation state is an effective strategy for the unification of the adsorption sites and reactive centers, which significantly improves the reaction kinetics and CO2 PRR efficiency. Taking advantage of the concept, we further propose p–p orbital hybridization between P atoms and the adjacent O atoms in BiVO4 at the interface constructed in the O-RP/BiVO4 Z-scheme heterostructure to create the oxidation state of RP. Theoretical calculations and spectral characterizations reveal that the interfacial atomic orbital hybridization lowers the CO2 activation energy barrier through the stabilization of the COOH* intermediate and facilitates the charge separation and transfer. Consequently, the optimized photocatalyst exhibits an excellent performance for sacrificial reagent-free CO2 PRR, with a production rate of 208 and 26.2 μmol g–1 h–1 for CO and CH4, respectively, ca. 21-fold higher than that of pristine RP and topping most of the hybrid photocatalysts with a noble metal as cocatalysts. This work provides critical insight for the design of high-efficiency photocatalysts for CO2 PRR.
研究领域:
材料科学
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环境科学
·
光催化
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产品关联
DOI
高影响因子
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