Journal of the American Chemical Society
·
2019
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IF 14.695
Ruijin Sun,Shifeng Jin,Lin Gu,Qinghua Zhang,Qingzhen Huang,Tianping Ying,YiRan Peng,Jun Deng,Zhiping Yin,Xiaolong Chen
The pairing of ions of opposite charge is a central principle of chemistry. Even though the ability to intercalate anions is desirable for many applications, it remains a key challenge for numerous host materials with their outmost layers beingn anions. In this work, we introduce a hydrothermal ion-exchange synthesis to intercalate oxidative S and Se anions between the Se layers of FeSe, which leads to single crystals of novel compounds (Se/S)x(NH3)yFe2Se2. In particular, the unusual anion–anion bonding between the intercalated S (or Se) and Se layers exhibits strong ionic characteristics. The charge transfer through the Se layer to S (or Se) intercalants is further confirmed by the elevated oxidation state of Fe ions and the dominant hole carriers in the intercalated compounds. By intercalating S, for the first time superconductivity emerged in hole-doped iron chalcogenides. The generality of this chemical approach was further demonstrated with layered FeS and NiSe. Our findings thus open an avenue to exploring diverse aspects of anionic intercalation in similar materials.
研究领域:
材料化学
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超导物理
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无机化学
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固态化学
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凝聚态物理
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高影响因子
Reaction Kinetics Mechanisms and Catalysis
·
2019
·Vol. 128
·期 2
·681-693
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IF 1.428
Xie Chong,Yang Shenghui,Shi Jian-Wen,Niu Chunming
A novel MnO x –TiO 2 catalyst with hollow silkworm structure was synthesized successfully via an ethanol-thermal strategy by using activated carbon fiber felt as template for the first time. The silkworm-like MnO x –TiO 2 catalyst (MnTi) exhibited higher NO x conversion in the whole experimental temperature region (90–330 °C) under a high space velocity of 36,000 h −1 in comparison with the common MnO x –TiO 2 catalyst without hollow silkworm structure (MnTi-B). The excellent catalytic performance of MnTi can be attributed to its high specific surface area, large content of active surface oxygen species (O S ), and more surface acid sites. In addition, the MnTi catalyst also exhibited excellent resistance to water or SO 2 poisoning.
研究领域:
催化化学
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环境科学
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ACS Sensors
·
2026
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IF 10.9
Zhang Xue,Sun Jiaxing,Wang Yuchen,Zhang Ziqi,Wang Duojia,Liu Kai,Tian Weiliang,Zhang Kewei
Atomically thin, two-dimensional (2D) semiconductors offer unprecedented opportunities for high-performance gas sensing, while the limited surface accessibility of their bulk counterparts severely restricts their practical applications. Herein, ultrathin graphitic carbon nitride (g-C 3 N 5 ) nanosheets with an average thickness of ∼1.7 nm were successfully synthesized via a facile and scalable sulfuric acid-assisted intercalation–exfoliation strategy using bulk g-C 3 N 5 derived from the thermal polymerization of 3-amino-1,2,4-triazole. The exfoliation process effectively tailors the electronic structure and maximizes the exposure of nitrogen-rich active sites, enabling enhanced surface adsorption and accelerated charge transfer. As a result, the as-prepared g-C 3 N 5 nanosheets exhibit outstanding room-temperature ammonia (NH 3 ) sensing performance, delivering a high sensitivity of 22.27 ppm –1 , a low detection limit of 27 ppb, and excellent selectivity under complex gas environments. Notably, the integration of g-C 3 N 5 nanosheets onto a flexible porous substrate further enables robust mechanical stability and efficient gas diffusion, supporting reliable operation under bending and long-term use. More importantly, the sensor demonstrates the capability to discriminate pulmonary infection patients from healthy individuals through exhaled breath analysis, highlighting its potential for non-invasive clinical diagnostics. This work not only provides an effective strategy for constructing high-performance carbon nitride-based gas sensors but also offers a promising platform for wearable healthcare monitoring and early disease detection.
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DOI
PubMed
高影响因子
Environmental Science-Nano
·
2023
·Vol. 11
·期 1
·309-323
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IF 7.3
Xin Liu,Xiang He,Zhi-Cheng Ma,Xi Xi,Shuang-Xi Wang
Organic ammonium salts which are formed from heterogeneous reactions are one of the important components of nitrogen-containing organic compounds (NOCs) in the atmosphere. In order to investigate the formation process of organic ammonium salts, a gas-flow system with the diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) technique was applied to monitor the influence of a simulated illumination on the heterogeneous reactions of toluene/O3/NH3 on hematite nanoparticles. The results revealed that toluene was transformed into benzoic acid under the action of oxidants (O3 and OH radicals). The carboxylic acid was neutralized with NH3 to form ammonium benzoate. The effect of light intensities on the reaction kinetics of ammonium benzoate formation from the heterogeneous reactions was also analyzed. With an increase in the light intensity from dark to 36 mW cm−2, the reaction rates increased from (1.20 ± 0.02) × 1018 ions per g s−1 to (2.30 ± 0.09) × 1018 ions per g s−1. This induced the formation of abundant active radicals, which accelerated the conversion of toluene to ammonium benzoate on hematite nanoparticles. However, the reaction rates decreased to (1.80 ± 0.03) × 1018 ions per g s−1 as the light intensity continued to increase to 100 mW cm−2. The yield of organic ammonium salts might be reduced owing to the volatilization of ammonium benzoate at a high light intensity. Meanwhile, the initial uptake coefficient showed a similar change trend. The values of the uptake coefficient increased by 81.1% when the light intensity increased from 0 mW cm−2 to 36 mW cm−2 but decreased by 21.1% when the light intensity increased from 36 mW cm−2 to 100 mW cm−2. Our results not only propose the heterogeneous reaction kinetics of toluene/O3/NH3 on the nanoscale hematite surface under different light intensity conditions, but also provide a theoretical support for further understanding the conversion process of volatile organic compounds (VOCs) under combined atmospheric pollution.
研究领域:
大气化学
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环境科学
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NEW JOURNAL OF CHEMISTRY
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2022
·Vol. 46
·期 45
·21730-21736
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IF 3.925
Ziyue Zhou,Renjiang Li,Ke Li,Kai Zong,Dongshun Deng
The efficient capture and separation of ammonia (NH3), a fundamental raw material as well as widespread pollutant, is significant in the fertilizer industry and for environmental protection protocols. In this work, several new type V deep eutectic solvents (DESs), composed of hydroxypyridine and phenol, were designed as efficient and reversible NH3 absorbents. All the DESs have low viscosity, good NH3 absorption performance and high NH3/CO2 selectivity. The optimal 3-hydroxypyridine/phenol (1 : 5) ratio could respectively capture 10.00 mol kg−1 and 4.63 mol kg−1 NH3 at pressures of 101.3 kPa and 10.0 kPa, better than most other DESs and ILs reported in the literature. The prepared DESs show satisfactory thermal stability and highly reversible absorption performance. By comprehensively analyzing the absorption behavior and spectroscopic results, the effective NH3 absorption ability of DESs was deduced being due to a relatively strong interaction between multiple weak acidic hydroxyl groups and basic NH3.
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CHEMICAL ENGINEERING SCIENCE
·
2022
·
IF 4.889
Wuyuan Liu,Zihan Gao,Ming Sun,Jiajian Gao,Lifeng Wang,Xiangyun Zhao,Runnong Yang,Lin Yu
A series of Cr α Mn β CeTiO x catalysts were prepared using one-pot precipitation method and evaluated for the selective catalytic reduction (SCR) of NO with ammonia. Among the catalysts prepared, the Cr 0.006 Mn 0.05 CeTiO x catalyst exhibited the highest low-temperature activity and widest activity window (＞90% NO conversion at 160–425 °C) as well as outstanding sulfur resistance. The catalysts were characterized using XRD, NH 3 /NO/SO 2 + O 2 -TPD, XPS, in situ DRIFT, and so on. The amorphous Cr 0.006 Mn 0.05 CeTiO x catalyst had a larger specific surface area, high ammonia adsorption and strong acidity, resulting in an improved catalytic activity. A high ratio of surface adsorption oxygen and Ce 3+ promoted the formation of NO 2 , a key intermediate gas in the fast SCR reaction. Furthermore, in situ DRIFT showed that the SCR reaction followed the Eley Rideal and Langmuir Hinshelwood mechanisms. Moreover, the synergetic effect of Cr and Mn inhibited the accumulation of hydrogen sulfate or sulfate considerably.
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高影响因子
JOURNAL OF POWER SOURCES
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2022
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IF 9.794
Dekun Shi,Zhaojun Shi,Lixin Zhang,Yaan Cao
A series of halogen ions (Cl − , Br − , or I − ) modified Bi 2 MoO 6 (Bi 2 MoO 6 –Cl, Bi 2 MoO 6 –Br, or Bi 2 MoO 6 –I) are synthesized via a one-step solvothermal method . It is determined that the halogen ions (Cl − , Br − , or I − ) are modified on the surface of Bi 2 MoO 6 as the -Bi-Cl, -Bi-Br, or -Bi-I species (the connected Bi 3+ is coordinated with three lattice O2- ions in Bi 2 MoO 6 ). The -Bi-Cl, -Bi-Br, or -Bi-I species on the Bi 2 MoO 6 surface can act as highly active sites to polarize and activate the N 2 and H 2 O molecules adsorbed on the surface of catalysts. Moreover, due to the surface-modified -Bi-Cl, -Bi-Br, or -Bi-I species, the visible light absorption is improved, the separation of photogenerated charge carriers is promoted, as well the band structure is better matched with the redox potential of photoreduction of N 2 . As a result, the photocatalytic activity of Bi 2 MoO 6 –Cl, Bi 2 MoO 6 –Br, or Bi 2 MoO 6 –I is improved for photoreduction of N 2 into NH 3 compared with Bi 2 MoO 6 . Overall, this work provides new insights into the doping states of halogen ions, the surface-active sites, the band structure, the photocatalytic activity, and the mechanism for photoreduction of N 2 into NH 3 for Bi 2 MoO 6 with modification of halogen ions (Cl − , Br − , or I − ).
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
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IF 8.128
Yifan Li,Yaqin Hou,Yongzhao Zhang,Yatao Yang,Zhanggen Huang
Surface interface regulation is an important research content in the field of heterogeneous catalysis. To improve the interface interaction between the active component and matrix, tremendous efforts have been dedicated to tailoring the morphology, size, and structure of composite catalysts. In this work, we report a confinement strategy to synthesize a series of core-shell catalysts loaded with metal oxides on titania nanotubes (TNTs), which were applied to the selective catalytic reduction of NO x with ammonia. Interestingly, the core-shell catalyst with confinement of TNTs exhibited the remarkable activity at low temperature region, N 2 selectivity and sulfur tolerance. Benefiting from the superior interfacial confinement characteristic of TNTs and Fe 2 O 3 , strong component interactions, the surface acid sites and strong oxidizability of MnO x were properly regulated, thus obtained the outstanding activity, N 2 selectivity and provide chemical protection to effectively prevent SO 2 poisoning. As far as the reaction mechanism, we found that the adsorption and reactivity of Lewis acid sites were the dominant factors affecting the activity in the NH 3 -SCR process by in situ DRIFT spectra. In general, our work provides an innovative strategy for constructing an TNTs-enwrapped nanocomposite with nano-confinement and core-shell structure to improve the low temperature SCR process.
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PubMed
高影响因子
JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
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2021
·
IF 5.541
Tingting Jia,Feng Zhou,Huixia Ma,Ying Zhang
The selectivity and stability of catalysts have always been a challenge in the field of catalytic fast pyrolysis (CFP). Herein, a series of waste animal bones collected from local market were employed as catalyst to convert biomass, with only acetonitrile and propionitrile in bio-oil, via catalytic fast pyrolysis and ammonization (CFP-A) process. Combined with characterization and control experiments of calcium-based components in bone, it was found that hydroxyapatite (HAP) was the catalytic active phase, while NaCl and KCl inorganic salts in bone inhibited the production of nitriles. Under the optimized conditions, the selectivity of acetonitrile and propionitrile from cellulose were 74.9 % and 25.1 % in bio-oil, respectively. Importantly, for the raw biomass, it still maintained high nitriles selectivity. The carbon yield of nitriles did not decrease after 10 cycles with HAP. Such a stable catalyst is first reported in the field of CFP, which is important for CFP to be economically sustainable.
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高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2020
·Vol. 55
·期 26
·12041-12052
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IF 3.553
Yi Xuerui,He Xiaobo,Yin Fengxiang,Yang Tong,Chen Biaohua,Li Guoru
The global NH 3 production is dominated by Haber–Bosch process, requiring high temperature and pressure. Electrochemical N 2 reduction reaction (NRR) under ambient conditions is a greener path for artificial N 2 fixation to NH 3 but calling for efficient catalyst to increase activity and selectivity. Herein, we report the iron-based metal–organic frameworks (MOFs), i.e., MIL-88B–Fe and amine-functionalized MIL-88B–Fe (NH 2 –MIL-88B–Fe) as efficient catalysts for electrochemical NRR under ambient temperature and pressure in neutral electrolyte. NH 2 –MIL-88B–Fe shows higher NH 3 yield rate of 1.205 × 10 –10 mol s −1 cm −2 than MIL-88B–Fe (3.575 × 10 –11 mol s −1 cm −2 ). Furthermore, NH 2 –MIL-88B–Fe exhibits the highest Faradaic efficiency of 12.45% at 0.05 V versus RHE. The control experiments prove that NH 3 is produced through electrocatalytic NRR. This work may trigger the interest of using MOFs as highly efficient catalysts for electrochemical NH 3 production.
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高影响因子
Catalysis Science & Technology
·
2020
·Vol. 10
·期 19
·6583-6598
·
IF 5.721
Jialing Chen,Gang Peng,Wei Zheng,Wenbo Zhang,Li Guo,Xiaoqing Wu
A superior Fe-containing MCM-22 zeolite prepared by a one-pot synthesis method (OP-Fe/M22) showed excellent NH3 selective catalytic reduction (NH3-SCR) activity and almost 100% N2 selectivity in a wide temperature window (200–500 °C). To investigate the effects of preparation strategies on the NH3-SCR reaction, other three Fe/MCM-22 zeolites with similar iron content (4.4–4.8 wt%) were prepared by solid-state ion exchange (SSIE-Fe/M22), incipient wetness impregnation (IM-Fe/M22) and mechanical mixing (MM-Fe/M22) methods, respectively. Catalytic results in NH3-SCR demonstrate that OP-Fe/M22 gives significantly higher activity in the whole temperature range (100–550 °C) than the other three post-synthesized catalysts. As revealed by XRD, UV-vis, H2-TPR, NH3-TPD, and Py-IR experiments, OP-Fe/M22 has the highest concentrations of isolated Fe3+ species and acid sites, and the lowest concentration of Fe2O3 nanoparticles among the four catalysts, which ensures its highest activity in the NH3-SCR reaction. Besides, OP-Fe/M22 exhibits the higher activity both in NH3 oxidation and NO oxidation reactions than IM-Fe/M22, indicating the better NO oxidation ability and NH3 storage capacity of OP-Fe/M22 which also facilitates the NH3-SCR process. In contrast with Cu-based MCM-22 zeolite obtained from the incipient wetness impregnation method at similar metal content (5% Cu/M22), OP-Fe/M22 shows comparable activity with 5% Cu/M22 in the low-temperature range (100–300 °C) while obviously higher activity at high temperatures (300–550 °C). Moreover, by removing part of undesired iron oxides in OP-Fe/M22 through mild acid post-treatments, the NH3-SCR activity of OP-Fe/M22 in the medium and high temperature ranges (200–550 °C) can be further improved, suggesting that OP-Fe/M22 is a potential catalyst with highly-efficient NH3-SCR activity in a wide temperature window.
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高影响因子
Journal of the Taiwan Institute of Chemical Engineers
·
2022
·
IF 5.477
Kaiwen Ni,Yuewang Peng,Geyu Dai,Huawang Zhao,Zhiwei Huang,Xiaomin Wu,Guohua Jing,Wei Feng,Ye Yuan
Background Ammonia bisulfate (ABS) deposition on the active sites of the catalyst surface is the main reason for SO 2 poisoning in low-temperature NH3-selective catalytic reduction (SCR). Accelerated ABS decomposition efficiently enhances the SO 2 resistance. Methods In this work, ceria was specifically chosen to decorate V 2 O 5 -WO 3 /TiO 2 catalyst (Ce-VW/Ti) to activate ABS decomposition in low-temperature NH 3 -SCR. Significant findings The optimal 7Ce-VW/Ti catalyst accelerated the decomposition of ABS and had superior SO 2 tolerance at 250°C. The additive CeO 2 improved the specific surface area and surface acidity, favoring the NH 3 -SCR catalytic activity. ABS was preferentially deposited on the additive CeO 2 on the surface of the 7Ce-VW/Ti catalyst and generated cerium sulfate, eventually protecting the active V 2 O 5 sites and TiO 2 support. Moreover, high quantity of V 5+ and charge transfer between active species V 2 O 5 and support TiO 2 could be maintained due to CeO 2 protection, subsequently maintaining the high NH 3 -SCR performance and enhancing the SO 2 tolerance.
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