SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
He Ma,Dashuai Li,Yingying Li,Yuanyuan Li,Changhua Wang,Xintong Zhang
While photocatalytic technology has been recognized as an effective means for removing low-concentration NOx in ambient atmosphere, it still faces the challenge of the deep oxidation in high efficiency. In many cases, the release of more toxic NO 2 byproduct appeared to be inevitable during the photocatalytic oxidation of NO. Herein we report that the atomically dispersed MnO x cocatalyst on TiO 2 (B) microspheres could significantly enhance the deep oxidation of NOx under mild photocatalytic conditions (1 mW/cm 2 UV-A light, 1 L/min flow rate). At an initial NO concentration of 0.35 ppm, ca. 67.15% of NO is oxidized on the MT-0.5 sample, which is 2.76 times higher than the pristine TiO 2 (B) sample. More importantly, the release of NO 2 is suppressed by 2.11 times. Comprehensive spectral analyses suggest that atomically dispersed MnO x effectively promotes the charge separation of photogenerated carriers in TiO 2 (B), even better than MnO x nanoparticles-loaded TiO 2 (B). EPR and in-situ FTIR analyses illustrate that atomically dispersed MnO x -loaded TiO 2 (B) sample exhibits excellent low concentration NOx abatement performance, thus providing a rational mechanism for the NO deep oxidation pathway. This study not only provides a unique approach for preparing non-noble metal atomically dispersed co-catalysts, but also affords an effective means for efficient photocatalytic NO degradation.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
Nanoscale
·
2024
·Vol. 16
·期 22
·10727-10736
·
IF 5.8
Peijiao Chen,Zhijun Li,Pengze Wang,Yuxin Yao,Tianwei Dou,Yang Qu,Liqiang Jing
The photocatalytic water-mediated CO2 reduction reaction, which holds great promise for the conversion of CO2 into valuable chemicals, is often hindered by inefficient separation of photogenerated charges and a lack of suitable catalytic sites. Herein, we have developed a glycerol coordination assembly approach to precisely control the distribution of atomically dispersed Cu species by occupying Ti-defects and adjusting the ratio between Cu species and Ti-defects in a hierarchical TiO2. The optimal sample demonstrates a ∼4-fold improvement in CO2-to-CO conversion compared to normal TiO2 nanoparticles. The high activity could be attributed to the Ti defects, which enhance the photogenerated charge separation and simultaneously facilitate the adsorption of water molecules, thereby promoting the water oxidation reaction. Moreover, by means of in situ EPR and FTIR spectra, we have demonstrated that Cu species can effectively capture photogenerated electrons and facilitate the adsorption of CO2, so as to catalyze the reduction of CO2. This work provides a strategy for the construction of atomic-level synergistic catalytic sites and the utilization of in situ techniques to reveal the underlying mechanism.
研究领域:
材料科学
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环境科学
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化学
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DOI
PubMed
高影响因子
CATALYSIS TODAY
·
2024
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IF 5.2
Wei Wang,Hong Zhao,Xikang Zhao,Junfeng Rong,Ning Liu,Peng Yu,Jingxin Xie,Genghuang Wu,Huan Li,Mudi Xin,Mingsheng Zong
Atomically well-dispersed platinum catalysts play a vital role in various chemical processes such as direct dehydrogenation of propane (PDH), due to their high performance originated from high atom utilization. However, these catalysts suffer from complex preparation methods, and preparing atomically dispersed Pt-based catalysts with feasible methods remains challenging. Herein, we report a convenient method to prepare efficient atomically dispersed Pt/C catalysts for PDH by sulfur doping into the carbon support by simple cyclohexane impregnation method. The prepared atomically well-dispersed catalysts possess strong interactions between Pt and carbon support, which led to improved exposure of active sites and higher propylene formation rate compared to that without sulfur doping. Sintering of the Pt species was also inhibited and stability was improved by 47%. Propylene selectivity also showed a positive correlation with the amount of sulfur doping. The propane conversion first increased and then decreased, which was due to the loss of sulfur during the reaction that caused the agglomeration of Pt and the evolution of structure. It was found that the maximum catalytic activity appeared with Pt clusters of ∼ 0.71 nm with an average Pt-Pt coordination number of 3.1 and Pt-Pt bond distance of 3.09 Å.
研究领域:
化学工程
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催化科学
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
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IF 9.7
Minghu Zhao,Junyi Chen,Fei Wu,Yungang Wang,Kai Chen,Chao Xiong,Rongshu Zhu
Rationally designing catalysts suitable for flue gas purification at low temperatures and unraveling the anti-poisoning mechanism at the atomic level remain challenges. Here, a highly dispersed Ni-doped MnO x catalyst (Ni 0.1 Mn 0.9 O x ) was constructed and applied for selective catalytic reduction (SCR) of nitrogen oxides (NO x ). The long-term stability of Ni 0.1 Mn 0.9 O x is up to 80% (180 ℃) after 18 h under SO 2 and H 2 O conditions. This is due to the fact that the highly dispersed Ni atoms enhance the redox and surface acidity of MnO x , and modulate the electronic structure of the active Mn sites. The denitrification reaction on Ni 0.1 Mn 0.9 O x mainly follows the Eley-Rideal mechanism. The anti-poisoning mechanism is that the introduction of Ni weakens the electron transfer between the Mn site and SO 2 , thereby inhibiting the adsorption of SO 2 . In particular, the H 2 O adsorbed on the Ni sites is decomposed to replenish the depleted Brønsted acid sites, which facilitates the adsorption of NH 3 . However, an excess of H 2 O can have an inhibitory effect. In addition, the mesoporous structure may increase the mass transfer rate and reduce the accumulation of harmful substances. This study provides viable insights for the design of SCR catalysts with excellent anti-poisoning ability.
研究领域:
环境科学
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催化化学
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DOI
PubMed
高影响因子
Nano-Micro Letters
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2025
·Vol. 17
·期 1
·1-14
·
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
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DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2017
·
IF 9.446
Fengliang Wang,Yingfei Wang,Yiping Feng,Yongqin Zeng,Zhijie Xie,Qianxin Zhang,Yuehan Su,Ping Chen,Yang Liu,Kun Yao,Wenying Lv,Guoguang Liu
The development of highly efficient photocatalysts with broad spectrum light response is a primary goal in the photocatalysis domain. Here we report on a novel ternary photocatalyst comprised of single atom-dispersed silver and carbon quantum dots, co-loaded with ultrathin g-C 3 N 4 (SDAg-CQDs/UCN), which exhibited a highly enhanced photoresponse and broad-spectrum (UV, visible, and near-infrared light) photocatalytic activity. The content of 1.0 wt% of CQDs and 3.0 wt% of Ag resulted in a 10-fold higher reaction rate than that of UCN under visible light irradiation. This improved broad-spectrum photocatalytic performance may be attributed to the surface plasmon resonance effect of Ag, up-converted fluorescent properties of CQDs, narrowed energy gap, as well as the electron separation and transfer capacity of both the Ag and CQDs. An electron spin resonance (ESR) technique, and reactive species (RS) scavenging experiments indicated that 1 O 2 and O 2 − were the dominant active species involved in the degradation of naproxen (NPX). Product identification and reaction site prediction revealed that the photocatalytic degradation of NPX included decarboxylation, hydroxylation, as well as the opening of the naphthalene ring. Mineralization experiments indicated that NPX and its degradation products would be finally transformed into CO 2 and H 2 O. Reactions in different water matrices indicated that SDAg-CQDs/UCN can be effectively employed for the degradation of NPX under ambient water conditions. Therefore, SDAg-CQDs/UCN offers a new strategy for the broad-spectrum utilization of solar light and provides a promising method for the remediation of water contamination.
研究领域:
环境科学
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材料科学
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光化学
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DOI
高影响因子
Materials
·
2020
·Vol. 13
·期 7
·1513
·
IF 3.057
Jialing Kang,Mengjia Wang,Chenbao Lu,Changchun Ke,Pan Liu,Jinhui Zhu,Feng Qiu,Xiaodong Zhuang
Due to the growing demand for energy and imminent environmental issues, hydrogen energy has attracted widespread attention as an alternative to traditional fossil energy. Platinum (Pt) catalytic hydrogen evolution reaction (HER) is a promising technology to produce hydrogen because the consumed electricity can be generated from renewable energy. To overcome the high cost of Pt, one effective strategy is decreasing the Pt nanoparticle (NP) size from submicron to nano-scale or even down to single atom level for efficient interacting water molecules. Herein, atomically dispersed Pt and ultra-fine Pt NPs embedded porous carbons were prepared through the pyrolysis of Pt porphyrin-based conjugated microporous polymer. As-prepared electrocatalyst exhibit high HER activity with overpotential of down to 31 mV at 10 mA cm−2, and mass activity of up to 1.3 A mgPt−1at overpotential of 100 mV, which is double of commercial Pt/C (0.66 A mgPt−1). Such promising performance can be ascribed to the synergistic effect of the atomically dispersed Pt and ultra-fine Pt NPs. This work provides a new strategy to prepare porous carbons with both atomically dispersed metal active sites and corresponding metal NPs for various electrocatalysis, such as oxygen reduction reaction, carbon dioxide reduction, etc.Keywords:platinum;atomically dispersed active site;nanoparticle;porous carbon;hydrogen evolution reaction
研究领域:
材料科学
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电化学
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DOI
PubMed
高影响因子
ACS Catalysis
·
2022
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IF 13.7
Rui Ma,Junxian Gao,Jiajing Kou,David P. Dean,Christian J. Breckner,Kaijun Liang,Bo Zhou,Jeffrey T. Miller,Guojun Zou
Nickel has been considered a promising nonprecious metal for propane dehydrogenation (PDH) because of its appealing ability to activate alkane molecules; however, synthesis of selective and stable Ni sites remains a challenge. Herein, we describe an alumina-supported isolated Ni(II) site by settling Ni2+ cations into Al3+ vacancy on γ-Al2O3 as a selective and stable Ni-based catalyst for PDH. Based on the results from combined characterizations, including in situ X-ray adsorption spectroscopy (XAS), scanning transmission electron microscopy (STEM), and in situ diffuse reflectance infrared Fourier-transform spectroscopy (DRIFTS), atomically dispersed Ni(II) sites with bonding to oxygen ions from the alumina support are demonstrated. PDH catalyst tests shows that the Ni(II) single-site catalyst delivers superior performance compared to a supported metallic Ni NP catalyst, possessing >93% propylene selectivity at considerable propane conversions (15–45%), which surpasses Ni nanoparticle (NP) catalysts. The correlation of selectivity to propylene on different Ni structures with the structural characterizations suggest that the coordinatively unsaturated tetrahedral Ni(II) sites facilitate the desorption of propylene, which inhibits the side reactions for coking. Moreover, the atomically dispersed Ni(II) sites remain in its local structure in the reaction-regeneration cycles, as evidenced by in situ XAS. This study on alumina-supported nickel catalysts affords insights into the nature of selective and stable nickel sites involved in the PDH reaction.
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
TALANTA
·
2024
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IF 5.6
Lulu Cui,Houshen Li,Weijie Shi,Yingying Jing,Shuhong Sun,Shiyun Ai,Zeyi Guo
Reducing the size of active species is a powerful means to improve the utilization rate of active metals and enhance the properties of bimetallic nanozymes. In this work, Fe was introduced into Ce-MOF through the coordination of Fe 3+ and organic ligands, and the coordination effect resulted in atomically dispersed Fe in the derived Fe/CeO 2 nanozyme. Due to the atomically dispersed Fe embedded in the lattice of CeO 2 , a large number of defect sites were generated, endowing the nanozyme with excellent peroxidase (POD)-like activity. The constructed total antioxidant capacity (TAC) sensor based on the POD-like activity of Fe 1.01 /CeO 2 nanozyme displayed a very wide linear concentration range for AA, Cys, Glu and Trolox. More importantly, this TAC sensor can be applied to the TAC detection in vitamin C tablets and beverages. This work provides theoretical guidance for the synthesis of high-performance bimetallic nanozymes for TAC detection.
研究领域:
材料科学
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生物医学
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DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2022
·Vol. 10
·期 10
·5580-5592
·
IF 14.511
Pui-Ching Poon,Yuanhao Wang,Weiqun Li,Dawson Wai-Shun Suen,William Wai Yan Lam,Denise Zi Jing Yap,B. Layla Mehdi,Jun Qi,Xiao-Ying Lu,Eugene Yin Cheung Wong,Chunzhen Yang,Chi-Wing Tsang
The development of low-cost, highly efficient and durable catalysts is the key to the practical use of ammonia borane as a promising storage material for on-board hydrogen production. Atomically dispersed metal supported catalysts not only maximize the efficiency of metal utilization, but they can also act as a robust support for metal nanoparticles. Herein, we report a facile synthesis of a type of carbon nanotube that consists of both Co nanoparticles and atomically dispersed cobalt single-atoms by direct carbonization of a mixture of cobalt-containing precursors and melem-C3N4. Our results suggested that Co nanoparticles were successfully embedded in the layers of graphitic carbon to effectively prevent them from aggregation and loss of catalytic activity. In addition, the Co single atoms greatly lowered the adsorption barriers of water molecules onto the catalysts for fast hydrolysis of ammonia borane. Interestingly, it was found that when the ratio of Co to melem-C3N4 was 1 : 33.3, the best reactivity and stability towards ammonia borane hydrolysis were achieved. The highest specific hydrogen generation rate can reach up to 7833 mLH2 gCo−1 min−1 at 40 °C, which far exceeded most of the non-noble metal catalysts for ammonia borane hydrolysis to date. The durability of the catalyst was successfully maintained for 40 cycling tests and no obvious decay was observed. The current study presents an example of how nanoparticles and single-atoms can be synergistically exploited for heterogeneous catalysis applications.
研究领域:
催化化学
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材料科学
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能源研究
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Jun Wan,Yang-Ai Ma,Yina Nie,Junhao Cheng,Chengming Wang,Lin Liu,Feng Fu
Photocatalytic selective aerobic oxidation in organic synthesis is a green and sustainable approach to producing valuable chemicals. However, the sluggish charge dynamics and limited active sites for O 2 activation tremendously hinder catalytic activity. Herein, we address these challenges by developing a novel polarization photocatalyst composed of atomically dispersed Ni sites with S-doped Bi 4 O 5 BrI (Ni/Bi 4 O 5 BrI-S), which demonstrates bulk-surface charge polarization and active site manipulation. Specifically, this bulk-surface charge polarization, resulting from a cascade of the bulk electric field (BEF) and local surface electric field (LSEF), induces efficient separation of bulk and surface charge carriers. Moreover, the atomically dispersed Ni sites substantially augment active sites for O 2 activation, further accelerating charge transfer and increasing the generation of photogenerated holes (h + ) and superoxide radical (•O 2 − ) active species for triggering efficient aerobic oxidation of sulfide. This study presents a collaborative strategy for manipulating charge behavior with potential applications in renewable energy and green chemistry.
研究领域:
材料科学
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有机合成
·
绿色化学
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产品关联
DOI
高影响因子
ACS Catalysis
·
2025
·
IF 13.1
Zhao Wang,Hao Yuan,Jian Tao,Shu-Lin Liu,Ying Hong,Zhi-Yi Hu,Jian Zhang,Bao-Lian Su
Semihydrogenation plays a key role in industrial hydrorefining of light alkenes, with a market above 400 billion by 2027. The high cost of commercial palladium-based catalysts strongly calls for innovation but with great challenges. Herein, copper nanoparticles decorated with a minimized ppm of Pd are developed through a chemical plating process to integrate the catalytic advantages of copper and palladium for achieving maximized catalysis in the semihydrogenation of a fatal impurity of butadiene in alkene feedstocks. The developed Pd–Cu catalyst (i.e., 114 ppm of Pd in Pd0.0033Cu1/TiO2) exhibits an unprecedented catalytic performance superior to commercial Pd/Al2O3, with 100% butene selectivity above 90% of butadiene conversion over 130 h on stream at 90 °C. Further exploration reveals that the atomically dispersed Pd on Cu nanoparticles, obtained at ultralow ppm levels of Pd loading, induces a hidden but critical H2 trap, which concentrates H2 on the Pd site for further H2 dissociation that offers intermediate hydrogen atoms to the tandem butadiene semihydrogenation over the third layer of Cu atoms neighboring Pd through hydrogen spillover. Moreover, a threshold on Pd density was identified at Pd/Cu surficial atomic ratio of 1/138 (i.e., Pd0.0033Cu1/TiO2) for maximizing butadiene semihydrogenation performance, based on an extreme collaboration between Pd for H2 dissociation and Cu for butadiene hydrogenation. This work provides important guidance for developing noble metal-saving catalysts in industrial applications.
研究领域:
催化化学
·
材料科学
·
工业化学
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）