RSC Advances
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2020
·Vol. 10
·期 15
·8709-8716
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IF 3.119
Lin Gu,Yunyun Dong,Yan Zhang,Bo Wang,Qing Yuan,Hongmei Du,Jinsheng Zhao
In this study, a nitrogen-containing ligand supramolecule named PPYTZ was successfully synthesized using 2,6-pyridinedicarboxylic acid chloride and 3,5-diamino-1,2,4-triazole in order to carry out oxygen reduction reaction (ORR). Such a polymer provides abundant coordination sites for iron ions, and the PPYTZ–Fe/C composite catalyst was formed with the PPYTZ–Fe complex loading on the surface of Vulcan XC-72 carbon. The physical characteristics and ORR performance of the composite catalysts were characterized systematically via various relevant techniques, and their catalytic activity and reaction mechanism were evaluated and compared. The results showed that the catalytic activities and the reaction mechanism of ORR were highly dependent on the formation of an Fe–N unit. Accordingly, the PPYTZ–Fe/C catalyst containing Fe–N active sites exhibited high ORR catalytic activity (an onset potential of +0.86 V vs. RHE) in 0.1 M KOH. Such an Fe–N catalyst can accelerate the adsorption of O2 and increase the limiting current density (from 2.49 mA cm−2 to 4.98 mA cm−2), optimizing the ORR catalytic process from a two-electron process to a four-electron process (an n value of 3.8).
研究领域:
材料科学
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电化学
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PubMed
高影响因子
Nature Energy
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2024
·
IF 49.7
Xu Zhanyou,Lu Ruihu,Lin Zih-Yi,Wu Weixing,Tsai Hsin-Jung,Lu Qian,Li Yuguang C.,Hung Sung-Fu,Song Chunshan,Yu Jimmy C.,Wang Ziyun,Wang Ying
The electrochemical CO 2 reduction reaction towards value-added fuel and feedstocks often relies on metal-based catalysts. Organic molecular catalysts, which are more acutely tunable than metal catalysts, are still unable to catalyse CO 2 to hydrocarbons under industrially relevant current densities for long-term operation, and the catalytic mechanism is still elusive. Here we report 3,5-diamino-1,2,4-triazole-based membrane electrode assemblies for CO 2 -to-CH 4 conversion with Faradaic efficiency of (52 ± 4)% and turnover frequency of 23,060 h −1 at 250 mA cm −2 . Our mechanistic studies suggest that the CO 2 reduction at the 3,5-diamino-1,2,4-triazole electrode proceeds through the intermediary *CO 2 –*COOH–*C(OH) 2 –*COH to produce CH 4 due to the spatially distributed active sites and the suitable energy level of the molecular orbitals. A pilot system operated under a total current of 10 A (current density = 123 mA cm −2 ) for 10 h is able to produce CH 4 at a rate of 23.0 mmol h −1 .
研究领域:
电化学
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催化
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可再生能源
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材料科学
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DOI
高影响因子
CHEMISTRY OF MATERIALS
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2024
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IF 7.2
Shichao Xu,Haifeng Wu,Yuanxi Liu,Zhen-Gang Wang
Recreating the intricate enzymatic sites within in artificial materials poses a significant challenge due to the complex folding characteristics of enzymes. In this study, we designed a supramolecular catalyst by assembling intramolecularly folding G-quadruplex DNA with Fmoc-amino acid aggregates and Cu2+. This supramolecular material possesses active sites and catalytic functions that rely on copper clusters, mirroring the functionality of catechol oxidase. Experimental and theoretical simulations showed that Fmoc-amino acids interact with G-quadruplex DNA through groove binding, facilitating Cu2+ coordination to both components, thereby enhancing the oxidative catalysis of Cu2+ upon assembly. Our catalyst exhibited excellent tolerance to high temperature, varying ionic strength, and extended room-temperature storage in aqueous solutions. Moreover, our supramolecular complex effectively catalyzed the degradation of doxorubicin, a drug with a high affinity for the DNA component, demonstrating its potential for removing pharmacological pollutants. Additionally, by integrating a photoisomerizable azobenzene derivative as a ligand to the G-quadruplex DNA, we can switch the activity of the enzyme-mimetic catalyst between on and off states by adjusting the irradiation wavelength. This multicomponent approach offers a promising avenue for the design and engineering of active, adaptable supramolecular catalysts.
研究领域:
生物化学
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材料科学
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纳米技术
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催化
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高影响因子
Nature Communications
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2024
·Vol. 15
·期 1
·1-10
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IF 14.7
Li Han,Xu Leitao,Bo Shuowen,Wang Yujie,Xu Han,Chen Chen,Miao Ruping,Chen Dawei,Zhang Kefan,Liu Qinghua,Shen Jingjun,Shao Huaiyu,Jia Jianfeng,Wang Shuangyin
Electrocatalytic C-N coupling from carbon dioxide and nitrate provides a sustainable alternative to the conventional energy-intensive urea synthetic protocol, enabling wastes upgrading and value-added products synthesis. The design of efficient and stable electrocatalysts is vital to promote the development of electrocatalytic urea synthesis. In this work, copper phthalocyanine (CuPc) is adopted as a modeling catalyst toward urea synthesis owing to its accurate and adjustable active configurations. Combining experimental and theoretical studies, it can be observed that the intramolecular Cu-N coordination can be strengthened with optimization in electronic structure by amino substitution (CuPc-Amino) and the electrochemically induced demetallation is efficiently suppressed, serving as the origination of its excellent activity and stability. Compared to that of CuPc (the maximum urea yield rate of 39.9 ± 1.9 mmol h −1 g −1 with 67.4% of decay in 10 test cycles), a high rate of 103.1 ± 5.3 mmol h −1 g −1 and remarkable catalytic durability have been achieved on CuPc-Amino. Isotope-labelling operando electrochemical spectroscopy measurements are performed to disclose reaction mechanisms and validate the C-N coupling processes. This work proposes a unique scheme for the rational design of molecular electrocatalysts for urea synthesis.
研究领域:
电化学
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催化
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材料科学
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化学工程
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PubMed
高影响因子
ACS Applied Materials & Interfaces
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2023
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IF 9.5
Junhong Liu,Haifeng Wu,Yuanxi Liu,Zhen-Gang Wang
We have engineered a colorimetric sensor capable of selective and sensitive detection of amino acids. This sensor employs a supramolecular copper-dependent oxidase mimic as the probe, stemming from our prior research. The oxidase mimic is constructed through the self-assembly of commercially available guanosine monophosphate (GMP), Fmoc-lysine, and Cu2+. It catalyzes the formation of a red product with a maximum absorbance at 510 nm. The changes in color and absorbance are responsive to both the concentrations and types of amino acids present. This effect is most pronounced in the presence of histidine, with a detection limit (LOD) of 6.4 nM. Furthermore, the catalytic probe can distinguish histidine from histamine and imidazole propionate, as well as 1-methyl-histidine from 3-methyl-histidine, based on their distinct coordination capacities with copper. This underscores the high selectivity of the sensing platform. Both theoretical simulations and experimental results (including UV–vis spectra, fluorescence, and EPR) indicate that the amino acids may engage in copper center coordination, thereby impeding O2 access to copper─a pivotal aspect of the oxidase catalysis. This sensing platform, characteristic of its swift response, simple fabrication, and exceptional sensitivity and selectivity, can also be applied to detect other biological analytes such as nucleotides. It holds potential for use in environmental and biochemical analyses.
研究领域:
分析化学
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生物化学
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传感器
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催化
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生物检测
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PubMed
高影响因子
Science Bulletin
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2023
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IF 18.9
Quanjun Tang,Liang Bai,Chen Zhang,Rongwei Meng,Li Wang,Chuannan Geng,Yong Guo,Feifei Wang,Yingxin Liu,Guisheng Song,Guowei Ling,Haitao Sun,Zhe Weng,Quan-Hong Yang
A dissolved-oxygen seawater battery (SWB) can generate electricity by reducing dissolved oxygen and sacrificing the metal anode at different depths and temperatures in the ocean, acting as the basic unit of spatially underwater energy networks for future maritime exploration. However, most traditional oxygen reduction reaction (ORR) catalysts are out of work at such ultralow dissolved oxygen concentration. Here, we proposed that the electronic axial stretching of the catalyst is essentially responsible for enhancing the catalyst’s sensitivity to dissolved oxygen. By modulating the lattice of iron phthalocyanine (FePc) as a model catalyst, the unique electronic axial stretching in the z -direction of planar FePc molecules was realized to achieve a boosted adsorption and electron transfer and result in a much improved ORR activity in lean-oxygen seawater environment. The peak power density of a homemade SWB using a practical carbon brush electrode decorated by the FePc is estimated to be as high as 3 W L − 1 . These results provide inspiring insights into the interaction between the catalyst and complicated seawater environment, and propose the electronic axial stretching as an effective indicator for the rational design of catalysts to be used in extremely lean-oxygen environment.
研究领域:
材料科学
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电化学
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能源存储
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PubMed
高影响因子
危险品化学品经营许可证（带存储）