INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Xiuquan Li,Ziqiang He,Congbo Li,Dugang Kang,Jie Chen,Youhong Wang,Fei Wang,Song Huang,Zhien Zhang
Aiming at the resource utilization of CO 2 and the value-added catalytic conversion of ethane, different reducibility oxide carriers were used to study. Through catalytic reaction experiments, catalyst characterization and kinetic analysis , the interaction between reducible carriers and active metals and their regulation on the catalytic reaction performance of ethane with CO 2 were revealed. Fe 1.5 Ni 0.5 /CeO 2 has the highest ethylene selectivity of 87% near 650 °C, and is a good catalyst for the CO 2 -assisted ethane oxidative dehydrogenation to ethylene reaction. The strong interaction between the reducible CeO 2 and ZrO 2 carriers and active metals makes the Fe–O–Ce and Fe–O–Zr covalent bonds on the Fe 1.5 Ni 0.5 /CeO 2 and Fe 1.5 Ni 0.5 /ZrO 2 catalysts stronger than Fe–O–Ti and Fe–O–Al covalent bonds on Fe 1.5 Ni 0.5 /TiO 2 and Fe 1.5 Ni 0.5 /γ-Al 2 O 3 catalysts. The lattice oxygen on the reducible catalyst is more readily involved in the reaction. The strong interaction between the active metal and the carrier results in the reduction of the FeO x species and the formation of new active sites, resulting in a high reactivity of the catalyst. The mutually promoted redox cycle between the active species Fe 3+/2+ -Ni 2+/0 and the reducible carrier variable metal Ce 4+/3+ species improves the catalytic performance for the reaction of ethane awith CO 2 .
研究领域:
化学工程
·
催化科学
✓ 已验证
DOI
高影响因子
CATALYSIS LETTERS
·
2011
·Vol. 142
·期 2
·195-204
·
IF 1.907
Yang Yifei,Jia Litao,Meng Yan,Hou Bo,Li Debao,Sun Yuhan
Abstract Ordered mesoporous carbon supported cobalt-based catalysts (Co/MC) were synthesized via incipient wetness impregnation with different amounts of furfuryl alcohol (FA) as carbon precursor. The characterizations of obtained Co/MC were subjected to N 2 adsorption, XRD, XPS, TEM, H 2 -TPR, H 2 -TPD and H 2 -TPSR. The results indicate that the reducibility and dispersion of Co active species vary significantly due to the difference of FA amount. By simply tuning the FA content from 25 to 100 wt%, the reduction temperature of deriving metallic Co shifts gradually to lower. The catalytic performance of Co/MC was evaluated for Fischer–Tropsch (FT) synthesis. The observed FT activity exhibits a volcano-type curve with the amount of FA due to the effect of both reducibility and dispersion of active species. As the precursor concentration overweighs 50 wt%, the ability of CO to dissociate over the active surface and the selectivity to the C 5+ products level off after experiencing an initial increase. Substantially, the catalysts with higher concentration of FA render the larger crystallites having an average size of more than 6 nm, which facilitates the CO hydrogenation by way of carbon chain propagation. It seems that the sample with FA content of 50 wt% is optimum in terms of FT activity and C 5+ selectivity. Graphical Abstract By simply tuning the carbon precursor furfuryl alcohol (FA) content from 25 to 100 wt%, the textural property of mesoporous carbon varies significantly, which further induces the different reducibility and dispersion of Co active species and the temperature of deriving metallic Co shifts gradually to lower. The catalytic performance of as-synthesized catalysts was evaluated for Fischer–Tropsch synthesis (FTS). The observed FT activity exhibits a volcano-type curve with the amount of FA due to the effect of both reducibility and dispersion of active species. At the FA concentration of support over 50 wt%, the selectivity to the C 5+ heavy molecular maintain invariant after experiencing an initial increase. It seems that the sample with respect to 50 wt% FA is optimum in terms of FT activity and C 5+ selectivity.
研究领域:
化学工程
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催化科学
✓ 已验证
DOI
高影响因子
FUEL PROCESSING TECHNOLOGY
·
2021
·
IF 7.033
Yane Zheng,Linzhou Zhao,Yajing Wang,Yuhao Wang,Hua Wang,Yaming Wang,Lihong Jiang,Xing Zhu,Yonggang Wei,Kongzhai Li
Chemical looping steam methane reforming (CL-SMR) is a promising pathway for producing syngas and hydrogen. A series of La 1-x MnCu x O 3 (x = 0, 0.05, 0.1, 0.15, 0.2) perovskites as the oxygen carriers were prepared via sol-gel method. The physicochemical properties of oxygen carriers were determined by XRD, BET, H 2 -TPR and CH 4 -TPR. Compared with the pure LaMnO 3 , La 1-x MnCu x O 3 oxygen carriers exhibited smaller crystal size and cell volume, and better reducibility . La 1-x MnCu x O 3 oxygen carriers also exhibited good oxygen mobility and high reactivity during the CL-SMR process. In the methane partial oxidation stage, the syngas productivity of La 1-x MnCu x O 3 (2.79–5.20 mmol/g) increased gradually with the Cu content. La 0.85 MnCu 0.15 O 3 and La 0.8 MnCu 0.2 O 3 showed higher CO selectivity and appropriate H 2 /CO ratio (1.92–2.10). In the water splitting stage, the H 2 contents over La 0.85 MnCu 0.15 O 3 and La 0.8 MnCu 0.2 O 3 began to decrease after the second cycles. However, the H 2 contents maintained at a relatively stable level during 3–11 cycles, suggesting a thermal stability. There was no CO formed in the water splitting step during 3–11 cycles, indicating better carbon formation resistance.
研究领域:
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
CATALYSIS LETTERS
·
2025
·Vol. 155
·期 10
·1-13
·
IF 2.4
Chen Shiqi,Huang Zhixuan,He Wentao,Wang Xinyu,Yang Zhiwei,Zhang Jing
Molybdenum nitride, because of the strong metal-support interaction between nitrogen and the metal, exhibits activity superior to that of bare metals, demonstrating its effectiveness as a co-catalyst to address the slow kinetics of the iron reduction in the Fenton process. Here, we introduced Mo 2 N as a co-catalyst to accelerate the cycles of Fe 3+ /Fe 2+ within a Fenton-like system consisting of Fe 3+ and H 2 O 2 , thereby enhancing the activation of hydrogen peroxide to generate reactive oxygen species (ROS). The system demonstrates excellent recyclability and stability. XPS spectroscopic analyses reveal that Mo(III) and Mo(IV) species on the Mo 2 N surface are capable of reducing free Fe(III), while FTIR analyses show nitrogen (N) and nitrogen oxide (NO x ) facilitate the adsorption and coordination of iron. Both homogeneous and heterogeneous reduced iron species are active in the activation of H 2 O 2 . EPR spectroscopy further confirms that the primary ROS generated are hydroxyl radicals (·OH) and superoxide anions (·O 2 − ). This study not only underscores the feasibility of Mo 2 N-based Fenton-like systems but also provides a new strategy for promoting the practical application of Fenton chemistry. Graphical
研究领域:
环境化学
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催化
·
材料科学
·
物理化学
·
分析化学
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2023
·
IF 11.4
Qing Cao,Biwu Chu,Peng Zhang,Qingxin Ma,Jinzhu Ma,Yuan Liu,Jun Liu,Yaqi Zhao,Hong Zhang,Yonghong Wang,Hong He
Nitrate photolysis is a vital process in secondary NOx release into the atmosphere. The heterogeneous oxidation of SO2 due to nitrate photolysis has been widely reported, while the influence of SO2 on nitrate photolysis has rarely been investigated. In this study, the photolysis of nitrate on different substrates was investigated in the absence and presence of SO2. In the photolysis of NH4NO3 on the membrane without mineral oxides, NO, NO2, HONO, and NH3 decreased by 17.1, 6.0, 12.6, and 57.1% due to the presence of SO2, respectively. In the photolysis of NH4NO3 on the surface of mineral oxides, SO2 also exhibited an inhibitory effect on the production of NOx, HONO, and NH3 due to its reducibility and acidic products, while the increase in surface acidity due to the accumulation of abundant sulfate on TiO2 and MgO promoted the release of HONO. On the photoactive oxide TiO2, HSO3–, generated by the uptake of SO2, could compete for holes with nitrate to block nitrate photolysis. This study highlights the interaction between the heterogeneous oxidation of SO2 and nitrate photolysis and provides a new perspective on how SO2 affects the photolysis of nitrate absorbed on the photoactive oxides.
研究领域:
大气化学
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环境科学
✓ 已验证
DOI
高影响因子
Catalysts
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2025
·Vol. 15
·期 3
·248
·
IF 4
Haichen Lai,Gaolei Shi,Liuwei Shen,Xingguang Zhang
As a type of sustainable and renewable natural source, biomass-derived 5-hydroxymethyl furfural (HMF) can be converted into high-value chemicals. This study investigated the interactions between silver (Ag) and oxide supports with varied reducibility and their contributions to tuning catalytic performance in the selective oxidation of HMF. Three representatives of manganese dioxide (MnO2), zirconium dioxide (ZrO2), and silicon dioxide (SiO2) were selected to support the Ag active sites. The catalysts were characterized by techniques such as STEM (TEM), Raman, XPS, H2-TPR, and FT-IR spectroscopy to explore the morphology, Ag dispersion, surface properties, and electronic states. The catalytic results demonstrated that MnO2with the highest reducibility exhibited superior catalytic performance, achieving 75.4% of HMF conversion and 41.6% of selectivity for 2,5-furandicarboxylic acid (FDCA) at 120 °C. In contrast, ZrO2and SiO2exhibited limited oxidation capabilities, mainly producing intermediate products like FFCA and/or HMFCA. The oxidation ability of these catalysts was governed by support reducibility, because it determined the density of oxygen vacancies (Ov) and surface hydroxyl groups (OOH), and eventually influenced the catalytic activity, as demonstrated by the reaction rate: Ag/MnO2(3214.5 molHMF·gAg−1·h−1), Ag/ZrO2(2062.3 molHMF·gAg−1·h−1), and Ag/SiO2(1394.4 molHMF·gAg−1·h−1). These findings provide valuable insights into the rational design of high-performance catalysts for biomass-derived chemical conversion.
研究领域:
催化化学
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生物质转化
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Surfaces and Interfaces
·
2024
·
IF 5.7
Jianfei Lei,Yanfei Liu,Ying Chen,Chenming Liang,Lele Wang,Yuan Cheng,Zexing Liang
Bimetallic single-atom catalysts have garnered substantial interest due to their extraordinary catalytic prowess, which arises from atomic-level synergistic effects that can significantly enhance hydrogen evolution reaction (HER) kinetics beyond the capabilities of monometallic single-atom catalysts. However, the fabrication of bimetallic single-atom catalysts remains a tremendous challenge. Herein, we introduce an in-situ reduction method to fabricate bimetallic single-atom catalysts anchored on hydrogenated molybdenum trioxide (H x MoO 3 , 0 < x ≤ 2). Intriguingly, H x MoO 3 exhibits inherent reducing capabilities that facilitate the in-situ reduction of some metal ions to metallic single atoms in steps on its surface, thereby enabling the constructing of bimetallic single-atom structures. As a testament to this strategy, the prepared PtM/H x MoO 3 catalysts (M = Ag, Au, Pd, Rh) with ultra-low noble metal loadings (wt% < 1%) on the nano-H x MoO 3 support exhibit remarkable efficiency in HER. Outperforming both monometallic single-atom catalysts (M/H x MoO 3 ) and commercial Pt/C, these catalysts demonstrate enhanced HER performance, and the PtPd/H x MoO 3 exhibits outstanding performance with an overpotentials of 10 mV at 10 mA/cm 2 , Tafel slope of 36 mV/dec, and long-term durability in acidic media. The presence of Pt single-atom significantly enhances the electrochemical surface area (ECSA) and accelerates the kinetics of the HER for other metal single atoms.
研究领域:
材料科学
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催化化学
·
能源化学
✓ 已验证
DOI
高影响因子
APPLIED MICROBIOLOGY AND BIOTECHNOLOGY
·
2018
·Vol. 102
·期 21
·9159-9170
·
IF 3.34
Mei Jingxia,Zhang Nan,Yu Yuanyuan,Wang Qiang,Yuan Jiugang,Wang Ping,Cui Li,Fan Xuerong
Proteases can cause unacceptable fiber damage when they are singly applied to wool anti-felting treatment which can make wool textiles machine-washable. Even if protease is attached by synthetic polymers, the modified protease plays a limited role in the degradation of keratin with dense structure consisting of disulfide bonds in the scales. Here, to obtain “machine-washable” wool textiles, a novel “trifunctional protease” with reducibility, hydrolysis, and localization is developed by means of covalent bonding of protease molecules with poly (ethylene glycol) bis (carboxymethyl) ether (HOOC-PEG-COOH) and l -cysteine using carbodiimide/N-hydroxysuccinimide (EDC/NHS) coupling, aiming at selectively degrading the scales on the surface of wool. The formation of polymer is confirmed with size exclusion chromatography (SEC) and Fourier transform infrared spectroscopy (FT-IR). Ellman’s test and fluorescence microscopy reveal that the modified protease can reduce disulfide bonds and restrict hydrolysis of peptide bonds on the wool scales. Furthermore, when applied to wool fabrics, the modified protease reach better treatment effects considering dimensional stability to felting (6.12%), strength loss (11.7%) and scale dislodgement proved by scanning electron microscopy (SEM), alkali solubility, wettability, and dyeability. This multifunctional enzyme is well-designed according to the requirement of the modification of wool surface, showing great potential for eco-friendly functionalization of keratin fibers rich in disulfide linkage.
研究领域:
生物化学
·
纺织科学
✓ 已验证
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2022
·
IF 8.047
Biyun Fang,Zeliang Qi,Fangming Liu,Chuanfeng Zhang,Chunyan Li,Jun Ni,Jianxin Lin,Bingyu Lin,Lilong Jiang
The development of efficient oxides-supported bimetallic catalysts is critical for ammonia synthesis or other catalytic reactions. Herein, the design of ceria-supported Co-Mo bimetallic catalysts with different properties is performed by changing Mo addition to enhance the ammonia synthesis activities. It is found that the reduction of ceria and molybdenum oxide would be boosted by Co species, but the reduction of the bimetallic catalyst would be inhibited by the aggregated molybdenum oxide for the catalyst with Co and Mo simultaneous addition. On the contrary, this ill effect of molybdenum oxide on the reduction of the bimetallic catalyst can be effectively alleviated by the subsequent addition of Mo species to ceria-supported Co catalyst, resulting in enhancement of the proportion of Co metal, Ce 3+ and low-valent Mo species, as well as surface enrichment of Co species. In such cases, the amount of the adsorbed hydrogen and nitrogen species would increase, and hydrogen species preferentially desorbs following a pathway of H 2 formation. As a result, the catalyst obtained by the separate addition of Co and Mo shows 2.5-fold more active than its counterpart with the simultaneous addition of Co and Mo species. These findings provide a valuable insight in designing reducible oxide-supported bimetallic catalysts in ammonia synthesis or other hydrogen-involved reactions.
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
高影响因子
FOOD CHEMISTRY
·
2021
·
IF 7.514
Ning Xiang,Sihong Wu,Zhengxun Wei,Ping Shao,Peilong Sun
Iron deficiency is a common nutritional disorder worldwide. Iron fortification of food is an effective strategy to control iron deficiency anemia (IDA), however, traditional iron fortificants usually provoke undesirable organoleptic changes or have limited colloid stability. In this research, we investigated iron reducibility of soy protein amyloid fibrils made from soy protein isolates (SPI), soy β-conglycinin (7S) and soy glycinin (11S), and explored their applications in iron fortification. All three protein fibrils showed iron reducibility. The reducibility was utilized to generate fibril-iron nanoparticle composites. The iron reducibility was affected by fibril concentration, degree of fibrillation and reducing amino acid composition. We identified 11S had the most significant effect on reducing Fe (III) to more bioavailable Fe (II) state, whereas 7S showed the optimal result for generation of iron nanoparticle on fibrils in situ . The resulted fibril-iron nanoparticle hybrids showed high dispersibility in various liquid foods, without distinct color change.
研究领域:
食品科学
·
营养学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2025
·Vol. 36
·期 19
·1-14
·
IF 2.8
Huang Shijun,Li Mulan,Chen Zehao,Yan Longlong,Liu Jingwen,Li Cai-Fu
The third-generation wide-bandgap semiconductor devices are supposed to be operated in a severe condition of high temperature. Die-attach bonding is also critical to realizing such high temperature operation. Cu particles paste has attracted considerable interest recently due to the superior conductivity and mechanical properties of copper. This work developed a long-time stable Cu paste with self-reducibility. The long-time stability can be attributed to the oxide passivation layer, the construction of physical barrier of polyethylene glycol 400 (PEG400) and the acid protection of ascorbic acid (AA). Additionally, both AA and PEG400 serve as reductants during the sintering process. AA initially reduces the oxides, while the reducing gases decomposed from PEG400 further enhance the reduction. Through combining the reduction process with the sintering process, in-situ generated fresh Cu nanoparticles with high surface energy can promote the necking growth of Cu grains, and lead to a stronger strength. In addition, it is revealed that the AA content, sintering temperature and sintering time play important roles in the sintering behaviors of Cu paste, thus affecting the mechanical and electrical properties of copper joints. The 2 wt.% AA joints that sintered for 5 min at 300 ℃ had an average shear strength of 43.91 MPa, which is 2.6 times higher than that of the bonding joints without AA. The utmost shear strength of 51.30 MPa and a low electrical resistivity of 8.85 × 10 –8 Ω m were achieved by sintering for 30 min. This long-term stable Cu paste paves the way for the wide application of Cu paste in power electronics.
研究领域:
材料科学
·
功率电子
·
半导体器件
·
纳米技术
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Kunli Song,Kaiyu Guo,Yixuan Lv,Dandan Ma,Yonghong Cheng,Jian-Wen Shi
Selective catalytic reduction with ammonia is the mainstream technology of flue gas denitration (de-NOx). The reducibility and acid site are two important factors affecting the de-NOx performance, and effective regulation between them is the key to obtain a highly efficient de-NOx catalyst. Herein, a series of Mn–Fe–BTC with different ratios of Mn and Fe are synthesized, among which 2Mn-1Fe-BTC with 2:1 molar ratio of Mn and Fe has excellent low-temperature (LT) de-NOx performance (above 90% NO conversion between 60 and 270 °C) and good tolerance to H2O and SO2 poisoning (88% NO conversion at 150 °C with 100 ppm of SO2 and/or 6% H2O). It is revealed that the reducibility properties and acid sites of Mn–Fe–BTC can be flexibly tuned by the ratio of Mn and Fe. The difference in electronegativity between Fe and Mn leads to the redistribution of valence electrons, which enables the controllable reducibility of Mn–Fe–BTC. Furthermore, different amounts of Mn and Fe lead to different electron transport, which determines the type and number of acid sites. The synergistic effect of Mn and Fe endows Mn–Fe–BTC with enhanced surface molecular adsorption capacity and enables the catalyst to selectively chemisorb NH3 and NO at different active sites. This research provides guidance for the flexible regulation of reducibility and acid site of LT de-NOx catalyst.
研究领域:
环境化学
·
催化
·
材料科学
·
大气污染控制
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）