Journal of Energy Chemistry
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2024
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IF 14
Hongqiang Yang,Jianfeng Zheng,Guoyu Wang,Yifei Gao,Yatao Yang,Jia Li,Xiaojin Han,Yan Cui,Zhanggen Huang
Photoelectrocatalytic coupling CO 2 and volatile organic compounds (VOCs) is a promising green strategy for the synergistic conversion of the two carbon-containing resources to C 2 products. The catalytic efficiency is always at the mercy of chemical inertness of CO 2 and the competitive hydrogen evolution of H 2 O. Herein, a modified g-C 3 N 4 /ZnAl-LDH Z-scheme heterojunction catalyst with dual reaction site was rationally designed and precisely constructed. The Faraday efficiency of ethanol reached 68.67% with a corresponding formation rate of 227.3 μmol g −1 h −1 . As revealed by in-situ characterizations and density functional theory calculations, CO 2 and HCHO were absorbed at Zn site and N site, respectively. Then, *CO generated from CO 2 and HCHO was converted to *CH 3 O and *CHO on the dual-active-site heterojunction. The detailed reaction mechanism experiments indicated that C–C coupling only occurred between *CO and *CH 3 O in electrocatalysis process. Apart from the “*CO + *CH 3 O” path, another “*CO + *CHO” coupling path was also detected in photoelectrocatalytic process. The selectivity of ethanol was significantly enhanced due to the synthesis of dual-site catalyst and the dual-path coupling path between CO 2 and HCHO simultaneously driven by light and electricity.
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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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Jingyi Wang,Guangzhi He,Chunying Wang,Xudong Chen,Xiaofeng Liu,Yaobin Li,Wenpo Shan,Hong He
Modulating the electronic metal-support interaction (EMSI) is one of the effective means to promote catalytic activity because it can adjust the electron occupancy of the d -band of noble metals, further facilitating the activation of reactants. Herein, we prepared a Pt/SiO 2 catalyst with an ultralow Pt loading of 0.05% and found that its catalytic activity in HCHO oxidation outperformed that of the Pt/TiO 2 counterpart, owing to the EMSI effect between Pt and SiO 2 . On this basis, the alkali metal Na was used as a promoter, and the formation of highly active Pt-O x (OH)-Na clusters enabled the complete oxidation of HCHO at room temperature. With ultralow Pt loading, the Pt-Na/SiO 2 catalyst reduces the cost of practical application remarkably. In situ DRIFTS and DFT calculations confirmed that the reaction pathways were distinct on Pt/SiO 2 and Pt-Na/SiO 2 . Specifically, on Pt-Na/SiO 2 , the reaction follows the mechanism of the direct degradation of formate species with the assistance of active hydroxyls; while on Pt/SiO 2 , CO is the only intermediate formed by the dehydrogenation of HCHO, due to the lack of active hydroxyls. These findings provide new insights into the reaction pathway of HCHO oxidation.
研究领域:
催化化学
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环境科学
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DOI
高影响因子
Inorganics
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2017
·Vol. 5
·期 4
·75
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IF 0
Zhixin Zhang,Yehong Wang,Jianmin Lu,Min Wang,Jian Zhang,Xuebin Liu,Feng Wang
We herein report the synthesis of 3-methyl-1,3-butanediol from isobutene and HCHO in water via a Prins condensation-hydrolysis reaction over CeO2, which is a water-tolerant Lewis acid catalyst. The CeO2exhibits significant catalytic activity for the reaction, giving 95% HCHO conversion and 84% 3-methyl-1,3-butanediol selectivity at 150 °C for 4 h. The crystal planes of CeO2have a significant effect on the catalytic activity for the Prins reaction. The (110) plane shows the highest catalytic activity among the crystal planes investigated (the (100), (110), and (111) planes), due to its higher concentration of Lewis acid sites, which is in line with the concentration of oxygen vacancies. Detailed characterizations, including NH3-TPD, pyridine-adsorbed FT-IR spectroscopy, and Raman spectroscopy, revealed that the concentration of Lewis acid sites is proportional to the concentration of oxygen vacancies. This study indicates that the Lewis acidity induced by oxygen vacancy can be modulated by selective synthesis of CeO2with different morphologies, and that the Lewis acidity and oxygen vacancy play an important role in Prins condensation and hydrolysis reaction.Keywords:CeO2;crystal plane effect;Prins condensation;hydrolysis;oxygen vacancy;Lewis acidity
研究领域:
催化化学
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材料科学
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DOI
CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Xueming Bao,Leilei Wu,Yuanyuan Yu,Bo Xu,Li Cui,Man Zhou,Qiang Wang,Ping Wang
Nowadays, with the rapid growth of population and acceleration of global urbanization, the microbial contamination on textiles and continuous formaldehyde (HCHO) releases from indoor decoration have aroused public attentions along with the textile consumption. Herein, a green, novel method for preparation of a multifunctional cotton fabric was reported, via the combination use of mussel-inspired fabrication of amine-quinone networks (AQN) and in-situ deposition of manganese dioxide (MnO 2 ). Unlike the conventional methods under extreme conditions, in this method, the MnO 2 particles were efficiently deposited on the fiber surfaces at room temperature within 30 min in the presence of reductive AQN surface composed of polyethyleneimine (PEI) and dopamine, and the MnO 2 -deposited cotton fabric exhibits efficient photothermal antibacterial capability against both Staphylococcus aureus and Escherichia coli , with inactivation efficiencies over 97% after 20 min of irradiation. In addition, this multi-functional fabric shows prominent UV-shielding property (UPF > 100) and HCHO purification ability, making 106.04 μg of HCHO rapidly removed within 30 min by 2.5 g of modified cotton. Therefore, we believe that the functional fabric exhibits wide applications in the fields of home textiles for antibacterial and air purification under mild conditions, and the special AQN structure can be further expanded to fabrications of other multifunctional nano-composites.
研究领域:
材料科学
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环境科学
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生物学
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DOI
高影响因子
JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2024
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IF 8
Jialin Liang,Fang Yuan,Ting Liu,Chenguang Qian,Zhangshuo Song,Lijuan Wei,Chunquan Li,Zhiming Sun
Photothermal catalytic oxidation is a promising and sustainable method for the degradation of indoor formaldehyde (HCHO). However, the excessively high surface temperature of existing photothermal catalysts during catalysis hinders the effective adsorption and degradation of formaldehyde under static conditions. Catalyst loading and oxygen vacancies (OVs) modulation are commonly employed strategies to reduce the photothermal catalytic temperature and enhance the efficiency of photothermal catalytic oxidation. In this work, a p-n type CuO/TiO 2 heterojunction is successfully loaded onto diatomite using a wet precipitation method. Under the irradiation of a 300W xenon lamp, the prepared composite material achieved a 100% removal rate of HCHO within 2 h, with a 98% conversion rate to CO 2 , surpassing the performance of both individual photocatalysts and thermocatalysts. Additionally, by adjusting conditions such as light irradiation and temperature, we have demonstrated that this material exhibits synergistic photothermal catalytic properties. Based on HRTEM, XPS, Raman, and EPR analyses, the introduction of diatomite as a catalyst support was shown to effectively increase the number of OVs. Experimental results, along with O 2 -TPD, photoelectrochemical characterization, and radical detection, demonstrate that the presence of OVs enhances the oxidative efficiency of both photocatalysis and thermocatalysis, as well as the UV–Vis-IR photothermal catalytic performance. The ternary composite material generates weak hydroxyl ( • OH) and superoxide ( • O 2 − ) radical under high-temperature with dark conditions, indicating its catalytic oxidation activity under this condition. The increase in temperature and the expansion of the spectral range both enhance the generation of these radicals. In summary, this work demonstrates that the use of diatomite as a support increases the material's specific surface area and OVs content, thereby enhancing adsorption and photothermal catalysis. It elucidates the enhanced catalytic degradation mechanism of this mineral-based photothermal catalyst.
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
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2026
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IF 12.5
Jing Wang,Hao Huang,Zhiguang Pan,Yan Zhao,Minghui Zhao,Tianqi Wang,Xinping Shi,Yanzhou Fan,Ying Yang
Developed a portable HCHO gas sensor for on-site detection. • Using MOF-derived strategy synthesize g-C 3 N 4 /Fe 2 O 3 /NiO ternary composite material. • The sensor exhibits excellent selectivity, repeatability, and stability. • The sensor successfully applied to the detection of residual HCHO in fresh shrimp. Formaldehyde (HCHO) is class 1 carcinogen. In the food supply chain, some vendors illegally use formalin (HCHO aqueous solution) to soak food products in order to extend their shelf life. Eating this food can increase the risk of developing malignant diseases such as leukemia and breast cancer. Therefore, it is crucial to develop portable sensors with high sensitivity, selectivity, and stability for HCHO detection. In this study, Fe/Ni-BTC derived Fe 2 O 3 /NiO nanoparticles are grown in situ on g-C 3 N 4 nanosheets, forming a unique g-C 3 N 4 /Fe 2 O 3 /NiO ternary composite. Gas-sensing test results indicate that the g-C 3 N 4 /Fe 2 O 3 /NiO sensor exhibits excellent gas-sensing performance at 240 °C to 50 ppm HCHO, including superior selectivity, high response (44.95), low theoretical detection limit (50.1 ppb) and long-term stability (60 days). We have further developed a portable HCHO detection system that has been successfully applied to detect residual HCHO in simulated aquatic products (fresh shrimp). This provides an effective monitoring approach to counteract the illegal use of HCHO for preventing food spoilage. It holds broad application prospects in the fields of environmental monitoring and food safety. Download: Download high-res image (162KB) Download: Download full-size image
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DOI
高影响因子
ENERGY & FUELS
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2025
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IF 5.3
Jinsong Luo,Tianci Xiao,Xiang Li,Qingyu Wang,Xusheng Zheng,Jiuzhong Yang,Chengyuan Liu,Yang Pan
The methanol-to-hydrocarbon (MTH) reaction offers a promising non-fossil fuel pathway for the production of olefins and aromatics. A formaldehyde (HCHO) intermediate has attracted great attention due to its critical role in the aromatization and coking process of the MTH reaction. However, because of the difficulty in the direct detection of HCHO, details on the impact of reaction condition on its formation and conversion were seldom studied. Here, synchrotron radiation photoionization mass spectrometry (SR-PIMS) was applied to thoroughly study the changes in HCHO and other relevant species under different reaction conditions, including contact time, temperature, zeolite acidity, and methanol concentration. It is revealed that higher temperature and acidity promoted the formation of HCHO and its transformation to aromatics and coke, whereas higher methanol concentration mainly enhanced hydrogen transfer reactions, resulting in a higher yield of polyunsaturated species and, consequently, more aromatics. Combining the results from SR-PIMS and soft X-ray absorption spectroscopy of the spent catalyst, it is verified that HCHO formation promoted coke formation, but the presence of olefinic species can shift the methanol conversion pathway toward methylation reactions and then limit the level of HCHO yield. Therefore, we proposed a butanol cofeeding strategy that can limit the contribution of HCHO-induced coke formation and extend the catalyst lifetime by up to ∼60%.
研究领域:
化学工程
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催化科学
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产品关联
DOI
高影响因子
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