ACS Catalysis
·
2022
·
IF 13.7
Xiao-Chen Sun,Kun Yuan,Wang-De Hua,Zi-Rui Gao,Qian Zhang,Chen-Yue Yuan,Hai-Chao Liu,Ya-Wen Zhang
The metal–support interface plays a crucial role in heterogeneous catalysis. The modulation of the metal–support interaction (MSI) affords the possibility of promoting the catalytic efficiency per active site. Here, we report a strategy to modulate the interfacial interaction and then optimize the interfacial activity of Co/CeO2 catalysts for the water–gas shift reaction (WGSR) by a facile NH3 treatment process for the CeO2 support. The sample of Co/800N-CeO2 treated at 800 °C exhibited the highest reaction rate of 260 μmolCO/(gCo s), which was 23.8 times higher than the rate of the untreated Co/CeO2 sample. A combination of ex situ and in situ characterizations suggested that addition of the NH3 treatment process did not only weaken the metal–support interaction between the Co species and CeO2 support to strengthen CO adsorption and CO activation ability but also induced oxygen vacancy generation under reaction conditions to accelerate H2O activation. Both worked together in promoting the catalytic efficiency for the WGSR via the carboxyl pathway at a low temperature. It was worth mentioning that the N species of the CeO2 support introduced by the NH3 treatment was removed after changing the catalyst structure under reaction conditions. The interfacial structure was robust in a 60 h test at 400 °C due to the coexistence mechanism of carboxyl and formate pathways avoiding the poisoning effect of formate species on the active sites. The construction of active interfaces could be extended to Fe/CeO2 and Ni/CeO2 catalysts and could bring great promise in the design of the interfacial structure of supported catalysts in wide applications including chemical transformation reactions and industrial catalysis.
研究领域:
催化化学
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材料科学
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能源化学
✓ 已验证
DOI
高影响因子
Journal of Water Process Engineering
·
2025
·
IF 6.7
Xianxian Sheng,Tianliang Wang,Guilu Zeng,Xiang Zhang,Mudassir Habib,Shuguang Lyu
In the advanced oxidation process (AOPs) induced by sodium percarbonate (SPC), reactive oxygen species (ROS) can be scavenged by a large amount of dissolved Fe(II) released within a short time. To address this issue, a slow-release Fe(II) process is proposed in this study, thereby enhancing the degradation of contaminants. SPC/Fe(III)/amorphous boron (B) and SPC/Fe(III)/citric acid (CA) procedures were employed to remove polycyclic aromatic hydrocarbons (PAHs), with B as the reductant and CA as the chelator. Fluoranthene (FLT) removal in SPC/Fe(III)/B process contributed to HO•, while HO• and O 2 − • were responsible for FLT degradation via SPC/Fe(III)/CA system. SPC/Fe(III)/CA system exhibits more adaptability to intricate water quality circumstances compared to SPC/Fe(III)/B system. The bio-toxicity of FLT and their degradation intermediates was evaluated via the Toxicity Estimation Software Tool (T.E.S.T.), revealing a reduction in oral rat LD50, developmental toxicity, mutagenicity, and bioconcentration factor of the degradation intermediates relative to FLT. Both amorphous B- or CA-assisted SPC/Fe(III) processes were shown to be eco-friendly through luminosity inhibition tests with Vibrio fischeri . Experiments on soil slurry revealed that SPC/Fe(III)/CA system was feasible for the removal of complex PAHs, directing the SPC-induced AOPs process for the remediation of PAHs contaminated soils and groundwater.
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DOI
高影响因子
CATALYSIS TODAY
·
2024
·
IF 5.2
Gongheng Zhang,Fengxiang Yin,Gideon Kofie,Qiuyue Gao,Jie Zhang,Guoru Li,Biaohua Chen
ZIF-67(CoFe) was synthesized using the solvothermal method , and the precursor of ZIF-67(CoFe)/xC-yIL was obtained by grinding the mixture of ZIF-67(CoFe), [BMIM][NTf 2 ] ionic liquid (IL), and carbon black. A series of ZIF-67(CoFe)/xC-yIL-T catalysts were prepared by calcining the precursor at different temperatures. The structure of the catalysts was examined using XRD , TEM, BET and XPS analysis. The results show that the high-temperature treatment of the precursor contributes to the formation of the structure of the N, S-co-doped carbon-coated nanoparticles . The introduction of ionic liquid increases the specific surface area of the catalysts and exposes more active sites. At the same time, as a sulfur source, ionic liquid forms a C-S bond, which is conducive to improving ORR activity. The optimal ORR half-wave potential and limited current density of ZIF-67(CoFe)/1.5 C-45IL-600 are 0.87 V vs. RHE and 4.64 mA cm -2 , respectively, in 0.1 mol L −1 KOH.
研究领域:
材料科学
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电化学
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纳米技术
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催化化学
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能量转换
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无机化学
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Qianlin Huang,Puzhen Zhao,Weiwei Wang,Lu Lv,Weiming Zhang,Bingcai Pan
Cost-efficient and durable manganese-based catalysts are in great demand for the catalytic elimination of volatile organic compounds (VOCs), which are dominated not only by the nanostructures but also by the oxygen vacancies and Mn–O bond in the catalysts. Herein, a series of nanostructured Co–Fe-doped-δ-MnO2 catalysts (Co–Fe-δ-MnO2) with high dispersion were in situ fabricated by employing metal–organic-frameworks (MOFs) as reducing agents, dopants, and templates all at the same time. The as-obtained Co–Fe-δ-MnO2-20% catalyst exhibited robust durability and high catalytic activity (225 °C) for toluene combustion even in the presence of 5 vol % water vapor, which is 50 °C lower than that of pristine δ-MnO2. Various characterizations revealed that the homogeneously dispersed codoping of Co and Fe ions into δ-MnO2 promotes the generation of oxygen vacancies and weakens the strength of the Mn–O bond, thus increasing the amount of adsorbed oxygen (Oads) and improving the mobility of lattice oxygen (Olatt). Meanwhile, due to successfully inheriting the framework structures of MOFs, the obtained catalyst exhibited a high surface area and three-dimensional mesoporous structure, which contributes to diffusion and increases the number of active sites. Moreover, in situ DRIFTS results confirmed that the toluene degradation mechanism on the Co–Fe-δ-MnO2-20% follows the MVK mechanism and revealed that more Oads and high-mobility Olatt induced by this novel method contribute to accumulating and mineralizing key intermediates (benzoate) and thus promote toluene oxidation. In conclusion, this work stimulates the opportunities to develop Co–Fe-δ-MnO2 as a class of nonprecious-metal-based catalysts for controlling VOC emissions.
研究领域:
环境科学
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材料科学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Liping Fang,Kai Wang,Chen Han,Xinyong Li,Pei Li,Jieshan Qiu,Shaomin Liu
Piezocatalysis utilizes mechanical energy to achieve the required charge separation for redox reactions, a promising method for clean H 2 O 2 production. However, the efficiency of conventional piezocatalysts is limited by the undesirable low piezoelectricity. Herein, novel piezocatalysts composed of La, Sr, Co (Fe) in simple single perovskites (La 0.5 Sr 0.5 FeO 3-δ and La 0.5 Sr 0.5 CoO 3-δ ) and Ruddlesden-Popper (R-P) type perovskites (LaSrFeO 4-δ and LaSrCoO 4-δ ) are developed for piezocatalytic H 2 O 2 production. Results indicate that Fe-containing catalysts outperform Co-containing counterparts and the unique R-P perovskite oxides demonstrate significantly enhanced piezocatalytic performance than the corresponding single perovskites. For example, via piezocatalysis, the LaSrFeO 4-δ exhibits H 2 O 2 yields of 548 (in 10 % ethanol) and 247 µmol g −1 h −1 (without sacrificial agent), improved by a factor of 1.14, 4.94, or 21.73 compared to La 0.5 Sr 0.5 FeO 3-δ , LaSrCoO 4-δ , or La 0.5 Sr 0.5 CoO 3-δ , respectively. The piezoelectricity is an overwhelming factor in determining the H 2 O 2 generation. Furthermore, the piezoelectricity and oxygen vacancy (OV) content is well correlated. The R-P phase with lower OV exhibits a higher piezoelectricity because of the eliminated pining effect to the polarization domain reversion. Mechanism exploration suggests that H 2 O 2 formation stems from the efficient O 2 reduction via a 2-electron transferring pathway, during which the piezoelectric polarization drives the charge separation and transportation, favoring the redox reactions.
研究领域:
材料科学
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环境科学
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化学
✓ 已验证
产品关联
DOI
高影响因子
Catalysis Science & Technology
·
2024
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IF 4.4
Zhicheng Xu,Jin Xiong,Yuran Li,Junxiang Guo,Bin Wang,Tingyu Zhu
For industrial flue gas purification at medium and low temperatures, it is highly necessary to promote the denitrification activity of V-based catalysts in a SO2 atmosphere. Transition metals (Ce, Co, Fe, and Mn) are used to modify V/Ti catalysts to improve SO2 resistance with ammonium bisulfate deposition on the catalysts. Sulfation on Ce with less ammonium bisulfate deposition considerably improves the SO2 resistance of V1Ce5/Ti, and stable sulfation on TiO2 promoted by Co provides additional Brønsted acid sites for V1Co5/Ti to reduce the deactivation. Serious sulfation on V1Mn5/Ti with large ammonium bisulfate deposition on V1Fe5/Ti causes deeper deactivation. The formation mechanism of ammonium bisulfate on active metal sites and TiO2 carriers has been clarified. SO2 is adsorbed on V sites and transition metal sites followed by oxidation and ammoniation or adsorbed on TiO2 carriers followed by ammoniation and oxidation. The first pathway is more dominant than the second pathway in the presence of O2 with the co-oxidation of SO2 by O2 and lattice oxygen. The initial formation temperature and stable temperature of dominant intermediates were determined by in situ DRIFTS. SO2 adsorbed on TiO2 carriers is oxidized by V sites above 170 °C to form a tridentate sulfate, while SO2 adsorbed on transition metal sites is initially oxidized by transition metal sites above 50 °C to form monodentate and bidentate sulfates, as well as competitively oxidized by V sites above 170 °C to form tridentate sulfates. The selective adsorption of SO2 on transition metal sites or TiO2 carriers and the competitive oxidation of SO2 by transition metal sites and V sites provide a synergistic effect between V sites and transition metal sites to reduce ammonium sulfate deposition and release more active sites. These findings provide theoretical guidance to design and prepare V-based catalysts with high denitrification activity in the presence of SO2.
研究领域:
环境科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Xing Yuan,Lingquan Meng,Chaohe Zheng,Haibo Zhao
Perovskites have been recognized as affordable substitutes for noble-metal catalysts for their tunable catalytic activity and thermal stability. Nevertheless, the highly demanding synthesis procedure still hinders the application of perovskites in catalytic combustion. In this work, a series of nanostructured SiTiO3 perovskites with B-site partial substitution by Co, Fe, Mn, Ni, and Cu are synthesized via flame spray pyrolysis in one step. The comprehensive characterizations on textural properties of nanostructured perovskites reveal that the flame-made perovskite nanoparticles all exhibit high crystal purity and large specific surface area (∼40 m2/g). Furthermore, the highest catalytic activity is achieved by SrTi0.5Co0.5O3 due to the formation of favorable oxygen vacancies, outstanding reducibility, and oxygen desorption capability. Additionally, the presence of 10 vol % water vapor during long-term testing indicates remarkable durability and water resistance. Finally, the CO oxidation and CH4 dehydrogenation on SrTiO3 incorporating Co atoms are more thermodynamically and kinetically favorable than those on other doped surfaces.
研究领域:
材料科学
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催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
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2022
·Vol. 47
·期 3
·1156-1164
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IF 3.925
Li-Jing Peng,Shi-Jun Yin,Li Chen,Tao Tian,Wei-Yi Zhang,Hang-Yu Zhou,Feng-Qing Yang
Herein, a Co–Fe Prussian blue analogue nanocube (Co–Fe PBA NC) was prepared in situ via a simple and rapid coprecipitation method at room temperature, and the synthesized nanocube was systematically characterized. The Co–Fe PBA NC was proven to have intrinsic oxidase-like activity, which can catalyze the production of reactive oxygen species, such as superoxide anions (O2˙−), hydroxyl radicals (˙OH), and singlet oxygen (1O2), in a dissolved oxygen system without the presence of hydrogen peroxide (H2O2). By making full use of the oxidase-like activity of the Co–Fe PBA NC and using the chromogenic substrate 3,3′,5,5′-tetramethylbenzidine (TMB), a colorimetric sensor was fabricated for the detection of ascorbic acid (AA) and its related biological enzymes’ activities, including alkaline phosphatase (ALP), α-glucosidase (α-Glu), and ascorbic acid oxidase (AAO), in human serum. This study presents an oxidase mimic that can be synthesized via a simple, rapid, and low-cost method, which overcomes the defects of cumbersome and time-consuming synthetic process, dependence on professional instruments and high cost of some previously reported nanozymes. In addition, this study provides a new multifunctional colorimetric sensing platform for AA and its related biological enzymes, showing great potential in biological assays.
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Sundaram Chandrasekaran,Na Li,Yang Zhuang,Lijun Sui,Zhizhong Xiao,Dayong Fan,Vanchiappan Aravindan,Chris Bowen,Huidan Lu,Yongping Liu
The creation of heterostructures based on non-precious metals with platinum-like hydrogen evolution reaction (HER) performance remains a challenge for hydrogen fuel technologies. Motivated by the fascinating properties of heterostructures, we establish here an effective approach to fabricate the heterostructured M−N−Ni 9 S 8 /Nb 2 O 5 ( M = Co, Fe, or Cu) catalysts using spatially separated Ni 9 S 8 nanosheet/Nb 2 O 5 nanobelts that are coupled with nitrogen (N) and metal atoms. Due to its improved intrinsic activity, interface-rich structure, abundant active sites, and large surface area the Co−N−Ni 9 S 8 /Nb 2 O 5 heterostructure achieved a low acidic HER overpotential of −171 mV at −10 mA cm −2 , thereby performing better than existing heterostructures. Moreover, for the alkaline HER, the Cu−N−Ni 9 S 8 /Nb 2 O 5 heterostructure required a low overpotential of −109 mV at −10 mA cm −2 , which is close to the performance of Pt/C catalyst. Density functional theory (DFT) predictions indicate that the local charge distribution and electronic properties at the heterointerface of Ni 9 S 8 /Nb 2 O 5 can be significantly modulated by co-doping of metals with N atoms, resulting in optimal adsorption energy and reduced water dissociation barrier; thereby accelerating the acidic and alkaline HER activity. This work, therefore, provides a new design principle to create advanced heterostructured catalysts.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
Surfaces and Interfaces
·
2024
·
IF 5.7
Cong Wang,Jingwei Li,Qingqing Wang,Jinze Cao,Jianjun Li,Liuyang Chen,Haibao Lu,Xiaodong He
The microscopic characteristics of carbon nanotube play a fundamental role in determining the macroscopic features. This research focuses on synthetic studies toward the structural evolution and microwave absorption enhancement of carbon nanotubes from biomass-based citric acid small organic molecules reaction system. When Co/Fe dual metal catalysts are used, self-entangled carbon nanotube networks in all three dimensions like instant noodles form. Polydimethylsiloxane (PDMS) is introduced inspired by “growth-from-template” strategy, the green hair algae-like morphology with bamboo-like structure is revealed in the carbon nanotubes. Twisted carbon nanotube yarn structure together with quaternary structure of protein-like carbon nanotube are both observed. Carbon microstructural evolution is investigated in bagasse-based ultralight composite. Toward the incident microwaves, in-situ synthesized CNTs-rGO composite has substantially enhanced reflection loss performance. The strongest reflection loss is -44.9 dB at 12.6 GHz with the absorber thickness of only 2 mm. And the effective microwave absorption bandwidth can reach 6.1 GHz covering a frequency range of 11.5–17.6 with the absorber thickness of only 1.6 mm.
研究领域:
材料科学
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纳米技术
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微波工程
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复合材料
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2024
·
IF 8.1
Shiqi Zhang,Ying Cheng,Zhiyuan Ni,Xuefei Lei,Biao Wang,Xuanwen Liu,Rui Guo
Reasonably designing and constructing transition metal based compounds with controllable composition and structure is a promising option for obtaining economically efficient oxygen evolution reaction (OER) electrocatalysts. This paper presents a one-pot self-templated epitaxial growth, phase transition and self-dissolution strategy for constructing hollow nanoboxes/solid nanocubes of CoFe bimetallic Prussian blue analogues (PBAs). The CoFe mixed phosphide with a porous hollow nanoboxes structure obtained after subsequent phosphating heat treatment exhibite enhanced OER electrocatalytic activity in alkaline media, exhibiting a low overpotential of 230 mV and a Tafel slope of 35.5 dec −1 at 10 mA cm −2 , as well as excellent stability for 48 h. The excellent OER activity of CoP-FeP nanoboxes (CoP-FeP NBs) can be attributed to the combination effect between their composition and structure. Structurally, the exquisite porous hollow nanoboxes structure greatly expands the surface area, reduces ion diffusion pathways, and reduces charge transfer resistance. Compositionally, the inner transition metal phosphide exhibits good conductivity and undergoes surface reconstruction during OER, forming high valence Co(Fe)OOH active substances in situ. The strong interface coupling effect of CoOOH/FeOOH optimizes the electronic structure. This work presents a facile and efficient strategy for the construction of PBAs hollow structural materials and the exploitation of low-cost and efficient electrocatalysts.
研究领域:
材料科学
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电化学
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纳米技术
·
催化
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）