Scientific Reports
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2017
·Vol. 7
·期 1
·1-8
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IF 4.259
Yang Yufang,Shen Dongjun,Long Yijuan,Xie Zhixiong,Zheng Huzhi
Ficin is classified as a sulfhydryl protease isolated from the latex of fig trees. In most cases, a particular enzyme fits a few types of substrate and catalyzes one type of reaction. In this investigation, we found sufficient proofs for the intrinsic peroxidase-like activity of ficin and designed experiments to examine its effectiveness in a variety of scenarios. Ficin can transform peroxidase substrates to colored products in the existence of H 2 O 2 . Our results also indicate that the active sites of peroxidase-like activity of ficin are different from that of protease, which reveals that one enzyme may catalyze more than one kind of substrate to perform different types of reactions. On the basis of these findings, H 2 O 2 releasing from MCF-7 cells was detected successfully. Our findings support a wider application of ficin in biochemistry and open up the possibility of utilizing ficin as enzymatic mimics in biotechnology and environmental monitoring.
研究领域:
生物化学
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酶学
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生物技术
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环境监测
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DOI
PubMed
高影响因子
ACS Applied Nano Materials
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2020
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IF 0
Meiling Fan,Xiangchuan Pan,Weiran Lin,Haining Zhang
Nitrogen-doped carbon materials are realized as effective electrode materials for oxygen-involved electrochemical devices. Understanding of active sites for adsorption of oxygen molecules is of significant importance for the development of carbon-based electrode materials. Herein, we synthesize two model catalysts named carbon-covered nitrogen-doped hollow carbon nanoparticles and nitrogen-doped carbon-covered hollow carbon nanoparticles by pyrolysis of block copolymer brushes to investigate the active sites for the adsorption of oxygen molecules. The electrocatalytic performance for oxygen reduction reaction (ORR) and carbon dioxide adsorption suggest that carbon atoms are Lewis basic active sites for oxygen adsorption. The coverage of a thin carbon layer on nitrogen-doped carbon materials can increase the surface density of Lewis basic sites for oxygen adsorption and can accordingly improve the electrocatalytic activity toward ORR as confirmed by a positive shift of both onset potential and half-wave potential.
研究领域:
材料科学
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电化学
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DOI
Nature Communications
·
2022
·Vol. 13
·期 1
·1-13
·
IF 17.694
Hao Jiace,Zhuang Zechao,Cao Kecheng,Gao Guohua,Wang Chan,Lai Feili,Lu Shuanglong,Ma Piming,Dong Weifu,Liu Tianxi,Du Mingliang,Zhu Han
High-entropy alloys have received considerable attention in the field of catalysis due to their exceptional properties. However, few studies hitherto focus on the origin of their outstanding performance and the accurate identification of active centers. Herein, we report a conceptual and experimental approach to overcome the limitations of single-element catalysts by designing a FeCoNiXRu (X: Cu, Cr, and Mn) High-entropy alloys system with various active sites that have different adsorption capacities for multiple intermediates. The electronegativity differences between mixed elements in HEA induce significant charge redistribution and create highly active Co and Ru sites with optimized energy barriers for simultaneously stabilizing OH * and H * intermediates, which greatly enhances the efficiency of water dissociation in alkaline conditions. This work provides an in-depth understanding of the interactions between specific active sites and intermediates, which opens up a fascinating direction for breaking scaling relation issues for multistep reactions.
研究领域:
材料科学
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电化学
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催化反应
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Xiaoli Yang,Yalan Wang,Haoxi Ben,Jia Yang,Wei Jiang,Anders Holmen,Yanqiang Huang,De Chen
Fischer–Tropsch synthesis over CoMn oxides is a surface-catalyzed structure-sensitive reaction. Active site changes greatly alter product distribution. The dynamics and essence of the changes in Co species during the reaction have seldom been explored. Herein, multiple characterizations were applied to confirm that two types of active sites, i.e., Co and Co 2 C, coexist on CoMnO x under the reaction conditions. Apart from the direct participation of carbon species in the reaction, the steady-state isotopic transient kinetic analysis also suggested the mutual transformation of carbon species in Co 2 C. The ratio of the two paths altered with the temperature, thus leading to Co 2 C-rich and Co-rich surfaces at intermediate and high temperatures, respectively. Kinetic calculations and microkinetic modeling showed that Co 2 C-rich surfaces facilitated CO adsorption and suppressed hydrogen adsorption. This gave high carbon-chain growth activity. The Co-rich surfaces showed high vacancy and hydrogen coverages, lowering the CO activation and CH 4 formation energies.
研究领域:
催化化学
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材料科学
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Xin An,Wei Jiang,Linhua Zhu,Lingchao Xu,Junfeng She,Jing He,Wenshuai Zhu,Huaming Li
Grain boundaries (GB), a favorable atomic configuration, can provide highly active surfaces by modulating electronic structures in the catalysts. Whereas, it is usually be ignored owing to the large structural variations and the difficulty in its precise design. Herein, a novel strategy is proposed to prepare nickel molybdate with rich GB (RGB-NMO) via a facile one-step growth assisted by cetyltrimethylammonium bromide. Experimental results reveal that the optimized morphology can increase the exposure of active sites and facilitate the mass transfer during the oxidative desulfurization (ODS) reaction. Moreover, the engineered GB can modulate the surface atomic composition and electronic structure, leading to the increase of hydrogen peroxide activation capacity. Benefiting from these features, the synthesized RGB-NMO not only exhibits attractive desulfurization efficiency, but also shows a satisfactory cycling stability. Overall, this manuscript provides new inspirations for design of functional materials rich in GB towards excellent ODS treatment.
研究领域:
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
ChemCatChem
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2024
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IF 3.8
Qi Yang,Ying Zheng,Yi Feng,Jie Ding,Maoshuai Li,Shouying Huang,Mei-Yan Wang,Xinbin Ma
Graphical Synergy between Rh 0 and Rh + on the Rh clusters is essential to catalyze heterogeneous formaldehyde hydroformylation. Rh 0 works as the adsorption/activation site for formaldehyde and hydrogen. Rh + works as the coordination site for CO and PPh 3 . The formed Rh─CH 2 OH* intermediate is responsible for the highly selective hydroformylation to glycolaldehyde. Controlling the metal geometric and electronic structure is of significance in developing efficient catalysts for heterogeneous hydroformylation. This study examines the structural sizes of Rh and Rh + -Rh 0 distribution to construct a highly active catalyst for formaldehyde hydroformylation. The active sites for hydroformylation require several Rh n atoms, while single-atom Rh can solely catalyze hydrogenation. The highest activity was achieved on Rh nanoclusters (0.95 nm), giving a TOF of 191 h −1 and selectivity of 82% for glycolaldehyde formation. The tunability of the electronic properties of Rh nanoclusters and the synergistic interaction between Rh + and Rh 0 are essential for enhanced activity. Pseudo- in situ FT-IR analysis elucidated that formaldehyde adsorbed on Rh nanocluster prefers to produce glycolaldehyde via hydroformylation, while formaldehyde adsorbed on isolated Rh δ+ sites tends to form methanol via hydrogenation. This study provides a new insight into the design of heterogeneous catalysts and guidance for understanding the reaction mechanism for aldehydes/olefins hydroformylation.
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
JOURNAL OF CATALYSIS
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2024
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IF 6.5
Cheng Liu,Huiling Chen,Qi Chen,Jinhong Bi,Jimmy C. Yu,Ling Wu
A series of Al 3+ -doped UiO-66(Ce) MOFs (U(Ce x Al 1−x )) was developed to reveal the roles of metal doping on active site formation and substrate activation in photocatalytic selective transformation of amines to imines. Al 3+ doping induced crystal structure distortion to form coordinately unsaturated metal (Al, Ce) sites as Lewis acid sites to chemisorb and activate benzylamine (BA). In situ FTIR revealed that the Al site with stronger acid strength facilitated BA activation. The activation degree of N–H bonds in BA was evaluated by changes of calculated force constant. The intermediate products were confirmed through time-dependent in situ FTIR. The Al 3+ -doped sample U(Ce 0.90 Al 0.10 ), the optimal catalyst, showed a significantly increased BA conversion (97.6 %) than that (47.5 %) of undoped sample, which was attributed to enough active sites and the optimal charge mobility. Finally, the present study proposes a synergistic photocatalytic mechanism associated with molecular activation to demonstrate selective oxidation pathways at the molecular level.
研究领域:
材料科学
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化学工程
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催化化学
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DOI
高影响因子
AICHE JOURNAL
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2025
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IF 4
Ziqi Bian,Minhao Chen,Xiaohu Ge,Ningchao Zhu,Yueqiang Cao,Hao Jiang,Jing Zhang,Gang Qian,Xinggui Zhou,Xuezhi Duan
Designing and fabricating uniformly dispersed non-precious metal active sites with tuned geometric configurations and local coordination environments for the selective conversion of functional groups to desired products is of great importance but remains challenging in industrial catalytic processes. In this work, we propose a straightforward method for synthesizing the Co 3 Sn 2 intermetallic catalyst through the structural conversion of layered double hydroxide precursors, thereby constructing suitable Sn-modified Co active sites and an optimized catalytic environment for propyne semihydrogenation. Characterizations using x-ray diffraction, high-resolution transmission electron microscopy, and x-ray absorption spectroscopy characterizations are combined to identify the formation of P6 3 /mmc Co 3 Sn 2 intermetallic phase. Catalytic performance tests show that the Co 3 Sn 2 catalyst achieves 95.0% propylene selectivity with nearly complete propyne conversion. Temperature-programmed surface reaction and desorption measurements combined with theoretical calculations demonstrate that the good selectivity is driven by the facile desorption of propylene from Sn-modified Co sites rather than its further hydrogenation.
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
APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
·
IF 20.2
Lihui Yang,Wenjian Yang,Shangtao Liang,Zeqin Lin,Jianxin Pan,Cao Yang,Tingting Zhu,Sihao Lv,Hui Lin
Nitrate electroreduction (NO 3 RR) is a promising alternative route for green synthesis of ammonia, where high-efficient catalysts are desired. Herein, an inexpensive ABO 3 -type perovskite BiFeO 3 was demonstrated as a highly efficient NO 3 RR catalyst compared to most of the reported non-precious catalysts. More interestingly, a surface evolution is observed in conjunction with an enhancement in NH 3 yield rate during the NO 3 RR process. Numerous metallic Bi 0 clusters and oxygen vacancies (OVs) are in-situ generated in the reconstructed BiFeO 3 (RS-BiFeO 3 ), and are proposed to be the genuine active sites. Density functional theory calculations suggest the RS-BiFeO 3 promotes the conversion of *NO 2 to *NO and enhances the *H supply for NO 3 - hydrogenation, thus boosting NO 3 RR. The yield rate of NH 3 by the reconstructed BiFeO 3 electrode reaches 5.3 mg cm −2 h −1 with a Faradaic efficiency of 86.8% at −0.7 V vs . RHE, over 4 times higher than that of the pristine BiFeO 3 electrode. This study establishes a fundamental understanding of BiFeO 3 reconstruction during NO 3 RR, and provides insights for the rational design of perovskite NO 3 RR electrocatalysts.
研究领域:
材料科学
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电化学
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催化
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Shuang Cao,Zhuoyi Zhang,Yunshuo Wu,Yuxin Sun,Zhe Li,Yanxia Gao,Haiqiang Wang,Xuanhao Wu,Zhongbiao Wu
Nitrous oxide (N 2 O) is a potent greenhouse gas with high global warming potential. It is urgent to develop active and stabile catalysts for N 2 O direct catalytic decomposition (deN 2 O) in industrial exhaust gas. In this study, a series of Eu-doped NiO catalysts were synthesized by co-precipitation method. The catalyst with an Eu to Ni molar ratio of 0.04 showed the highest deN 2 O ability, reaching 100 % conversion at 400 °C without generating NO x by-products. The catalyst also displayed resilience against O 2 and NO impurity gases, maintaining structural stability and achieving complete transformation of N 2 O at 440 °C. Eu was uniformly dispersed in NiO in the form of Eu 2 O 3 , which not only regulated the particle size and specific surface area of NiO, but also changed the surface chemistry of NiO by inducing more Ni 2+ active sites and more mobile O β species. Eu-doping altered the decomposition mechanism of N 2 O from L-H to E-R mechanism, reducing the energy barrier of O 2 desorption, which was the rate-determining step. During the reaction, Eu 0.04 Ni showed an activation behavior after cyclic use and long-term reaction and reduced T 100 to 320 °C after 14-hr experiment. These findings demonstrate the potential of the catalyst for practical application and provide new routes for the direct decomposition of N 2 O in industrial exhaust gas.
研究领域:
环境科学
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催化化学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
·
IF 9.7
Yue Sun,Xiang Li,Bin Du,Jialong Cui,Ali Abdullah,Yanji Zhu,Huaiyuan Wang,Di Bao
Global warming is attributed to excessive emissions of greenhouse gases, which are being addressed through the deployment of carbon capture technologies aimed at mitigating climate change. However, this approach faces significant challenges, as high concentrations of CO 2 pose a huge risk of corrosion, compromising integrity. The active inhibitor polyfluoroaniline grown on the surface of graphene (Gr-PFAN) is encapsulated in epoxy novolac (EN) coating. And highly reactive nitrogen-containing poly(p-phenylenediamine-fluoroaniline) (Gr-PPFAN) was synthesized by changing the polymerization monomer. For the first time, primary amine nitrogen-containing active sites are discussed in CO 2 shielding material. The gas transmission rate (GTR) test showed that the GTR of the composite film containing Gr-PPFAN was 3.7 times higher than that of Gr-PFAN. And the presence of highly reactive amines in the polymer mass transfer behavior was calculated by molecular simulation. Therefore, the PPFAN coating is a serious failure in H 2 O-CO 2 environment. The introduction of the low content of active sites in Gr-PFAN into the epoxy resin matrix resulted in significant enhancement of the H 2 O, H 2 O-CO 2 and H + corrosion resistance. The small amount of active amine not only enhances the phase interface between the resin and the flake filler, but also facilitates the formation of a protective layer on the metal surface. Experimental results demonstrated that Gr-PFAN/EN exhibited the highest |Z| 0.01 Hz value (3.5 × 1011 O × cm 2 ) after 90 days of immersion in 3.5 wt% NaCl solution and 1.5 × 1011 O × cm 2 for 30 days in the carbon capture environment. Furthermore, it makes Gr-PFAN/EN a promising candidate for practical applications in CO 2 capture projects. The findings provide a scientific basis for the development of efficient anti-corrosion coatings suitable for carbon capture technologies.
研究领域:
材料科学
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环境科学
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产品关联
DOI
PubMed
高影响因子
Nano-Micro Letters
·
2025
·Vol. 17
·期 1
·1-14
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IF 36.3
Zhong Yihong,Yuan Guotao,Bao Dequan,Tao Yi,Gao Zhenqiu,Zhao Wei,Li Shuo,Yang Yuting,Zhang Pingping,Zhang Hao,Sun Xuhui
The heteroatom atomically doping strategy was reported to construct highly
efficient sites on metal oxides for the detection of low-concentration gas.
The atomically dispersed Sn atoms were intentionally incorporated into the Fe 2 O 3
lattice during the oxidative annealing of Fe-based metal organic framework,
leading to specific Sn–O–Fe sites, porous structures, and abundant oxygen
vacancies.
The optimized Sn-Fe 2 O 3 exhibited exceptional sensing performance for NO 2
detection: ultra-high sensitivity ( Rg / Ra =2646.6 to 1 ppm NO 2 ), ultra-low limit of
detection (10 ppb), and high selectivity.
研究领域:
材料科学
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环境监测
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化学传感器
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）