NANO
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2019
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IF 1.293
Qian Sun,Chun Zeng,Meng-Meng Xing,Bo Chen,Dan Zhao,San-Guo Hong,Ning Zhang
Deliberately engineering oxide composites on constructing and manipulating interactive structures particularly in surface layers was highly desirable for heterogeneous catalysis. Herein, upon the redox replacement reaction between Ce(IV) precursor (Ce(NO 3 ) 6 2 − ) and Cu 2 O nano-substrate, an attempt to directly engineer the surface structure of Cu-based substrate was performed by the Ce(IV)–Cu 2 O etching-embedding process, then the obtained powders were thermo-treated to get a series of Ce–O–Cu catalysts with different Ce:Cu molar ratios for NH 3 selective catalytic reduction (NH 3 -SCR) of NO. Characterized by ICP-OES, XRD, Raman, XPS, SEM, BET, H 2 -TPR, NO- and NH 3 -TPD measurements, it was demonstrated that the Cu–O–Ce catalysts were structured as CuO matrix with an interactive surface composed by co-present Cu(I)–Cu(II) and Ce(III)–Ce(IV) species, even the introduction of Ce was confined in a quite low loading range (0.83–2.3 wt.%); such a surface exhibited the distinct synergistic effect with positively manipulated physical-chemistry properties such as active site distributions, redox features and surface reactivity compared to pure CuO and traditional Cu–Ce composite catalyst, leading to attractive catalytic performance such as ≥ 9 0 % NO conversion with ≥ 9 5 % N 2 selectivity and the two-fold TOF enhancement versus traditional catalysts, even SO 2 was present in reactant mixture on well-manipulated catalyst (Ce loading at 1.6 wt.%) These results indicated that the etching-embedding strategy illuminated in this work could be referred as a feasible method to directly engineer and construct interactive oxide composite surface for advanced application as well as current efficient Ce–O–Cu catalytic interface for heterogeneous catalysis.
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高影响因子
APPLIED CATALYSIS A-GENERAL
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2019
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IF 4.63
Li Cao,Xiaodong Wu,Ze Chen,Yue Ma,Ziran Ma,Rui Ran,Zhichun Si,Duan Weng,Baodong Wang
CeO 2 /WO 3 -TiO 2 (CeWTi) and Nb 2 O 5 -CeO 2 /WO 3 -TiO 2 (NbCeWTi) catalysts were prepared by a sol-gel precipitation method. Both the catalysts exhibit high selective catalytic reduction of NO x with NH 3 (NH 3 -SCR) activities at 270–500 °C. The sulfur tolerances of the catalysts were evaluated at 270 °C by adding H 2 O and SO 2 in the feeding gas and NbCeWTi exhibited a significantly improved resistance. The thermogravimetric (TG) and mass spectrographic (MS) results indicated that much less sulfates formed on NbCeWTi and existed mainly in the form of ammonium hydrogen sulfate species which protected Ce x+ active sites effectively from attacking of SO 2 . According to the results of temperature-programmed desorption of ammonia (NH 3 -TPD), H 2 temperature-programmed reduction (H 2 -TPR) and SO 2 oxidation , loading niobia on CeWTi inhibited the SO 2 oxidative adsorption and SO 3 production which basically reduced sulfur poisoning of the catalyst. Additionally, the niobia modification ensured the formation of nitrates from the competitive adsorption of SO 2 and hereby facilitated the nitrate SCR route based on the in situ diffuse reflectance infrared Fourier transform spectra (DRIFTS).
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高影响因子
APPLIED CATALYSIS A-GENERAL
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2017
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IF 4.339
Baohuai Zhao,Rui Ran,Xingguo Guo,Li Cao,Tengfei Xu,Ze Chen,Xiaodong Wu,Zhichun Si,Duan Weng
Mn/Ce/Ti and Mn/Ce/Nb/Ti catalysts were synthesized using a precipitation method and their catalytic activities for NO selective reduction with NH 3 at low temperatures were evaluated. Nb doping not only improved the activity of the catalyst over a wide temperature range but also restricted the generation of NO 2 and N 2 O. The Mn/Ce/Nb/Ti catalyst displayed 100% NO conversion from 150 to 250 °C and >90% N 2 selectivity below 250 °C. The specific surface area of the catalyst was increased and its surface acidity was strengthened after Nb doping. Moreover, Nb doping increased the NO oxidation ability and lowered the NH 3 oxidation activity of the catalyst. All the above factors contributed to enhancing the overall NH 3 -SCR performance of the Mn/Ce/Nb/Ti catalyst compared with that of the Mn/Ce/Ti one. The long-term stability and resistance to H 2 O and SO 2 of the Mn/Ce/Nb/Ti catalyst were also evaluated.
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高影响因子
ACS Applied Materials & Interfaces
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2024
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IF 8.3
Xinmiao Nie,Xue Zhong,Fan Yang,Rongguo Wang,Xiaodong He,Wenbo Liu
Real-time detection of harmful gases at room temperature has become a serious problem in public health and environmental monitoring. Two-dimensional materials with semiconductor properties BiOCl is a promising gas-sensitive material due to its large specific surface area and adjustable band gap as well as outstanding safety characteristics. However, limited by the weak gas adsorption sites and sluggish charge-transfer ability, the performance of BiOCl could not be fully exploited. Oxygen vacancy (Vo) engineering can introduce lattice defects, thereby significantly increasing the local charge density and enhancing the adsorption of gases, which is an effective strategy to enhance the gas-sensing performance. In this work, we composite BiOCl with a vacancy (Vo-BiOCl) and reduced graphene oxide (rGO) to construct a Vo-BiOCl/rGO heterostructure with enhanced gas adsorption sites. Experimental and theoretical calculations show that Vo can enhance the adsorption of gases and the introduction of rGO forms a high-quality heterostructure with BiOCl, which can effectively reduce the band gap of BiOCl and promote electron transfer, thereby improving the sensitivity of the sensor. Benefiting from above, Vo-BiOCl/rGO achieves the ability to detect low concentrations of NO2/NH3 at room temperature, with high sensitivity (55% at 1 ppm of NO2 and −28% at 1 ppm of NH3), fast response time (40 s at 1 ppm of NO2 and 2 s at 1 ppm of NH3), good stability (over 150 days), and fully recoverable gas sensitivity.
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PubMed
高影响因子
APPLIED ENERGY
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2024
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IF 10.1
Fawei Lin,Chujun Luan,Huiyi Mao,Chenxu Zhong,Xinlu Han,Guanyi Chen,Lei Che
The petroleum industry and pyrolysis of organic solid waste produce a large amount of low-grade fuel oil characterized by high proportions of heavy fractions, unsaturated compounds, and oxygen content. Catalytic hydro-pyrolysis is an effective approach to improve the quality with co-production of valuable pyrolysis gases and high-grade pyrolysis oils. However, exploration of available and low-cost hydrogen donors is the determining factor for the feasibility of this technique. Given that NH 3 is the excellent hydrogen carrier and with an active molecular structure, this work innovatively proposed NH 3 assisted catalytic pyrolysis that could significantly promote hydrogenation and cleavage reactions to acquire high-quality products and efficient utilization of NH 3 energy. HZSM-5 with specific modification by desilicication and phosphorus loading was selected as the optimal catalyst. The abundant hierarchical pore structure and weak acidity mainly contributed to the excellent catalytic performance. Specifically, 3 + rings aromatics (≥3 rings) disappeared, long-chain alkanes decreased by 10.45 %, while short-chain alkanes increased from 0 to 42.05 % for HO pyrolysis at 550 °C. The stability and universality of this approach were respectively investigated. Meanwhile, the heat value of pyrolysis gas increased by 3766 times under the optimal condition mainly due to the distinctly high yield of C 2 -C 4 combustible hydrocarbons, ca. 429.22 mL/g-oil. Accordingly, the pyrolysis gas could reach the target of energy self-supply for pyrolysis process by in-situ combustion with the residual NH 3 . Additionally, simulation calculations demonstrated that co-combustion of NH 3 and pyrolysis gases increased the laminar burning velocity and enhanced the combustion efficiency of NH 3 . Approximately 37,675 kJ/kg-oil energy could be produced in gas during NH 3 assisted catalytic pyrolysis to provide sufficient heat in pyrolysis with zero natural gas input. Extremely low production of CO 2 , zero natural gas input, and abundant C 2 -C 4 hydrocarbons jointly promoted the negative carbon effect, ca. 948.65 L CO 2 -eq./kg-oil. This study aims to propose NH 3 as a hydrogen donor so that low-grade fuel oil can be upgraded with energy self-supply.
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高影响因子
CHEMICAL ENGINEERING SCIENCE
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2024
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IF 4.1
Yuting Hu,Minghu Zhao,Bo Du,Ting Cheng,Zhaozhong Jiang,Kai Qin,Chengzhu Zhu
A series of M-MnCeO X catalysts using MOF (Metal-organic Framework) were prepared to apply for NH 3 -SCR (Selective Catalytic Reduction) of NO X . The effects of Mn/Ce molar ratio, calcination temperature and its activity including catalytic activity, H 2 O/SO 2 resistance and stability were systematically investigated. The results showed that under the Mn/Ce molar ratio of 1 and calcination temperature of 400 ℃, the catalyst exhibited excellent catalytic activity, H 2 O/SO 2 resistance, and stability. When the concentration of NO was 500 ppm, the gas spatiotemporal velocity (GHSV) was 36,000 h −1 , and the reaction temperature was 100 ℃, the NO conversion efficiency of M-MnCeO X exceeded 90.0 %. Added 200 ppm SO 2 and 3 vol% H 2 O simultaneously, the NO conversion efficiency was close to 80.0 %. By analyzing the physicochemical properties of the catalyst, M-MnCeO X had a large specific surface area, numerous acidic sites, and excellent redox properties. According to density functional theory (DFT), the NH 3 /NO adsorption energy of M-MnCeO X were −2.35 and −2.40 eV, exhibiting lower than a single MOF-derivative, promoting the adsorption of NH 3 or NO. The reaction mechanism on the M-MnCeO X catalyst followed the E-R and L-H mechanisms by In situ DRIFTS.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Tianren Liu,Wensheng Zhang,Qingmei Tan,Weilong Lian,Haiting Lin,Jianshen Li,Dongxue Han,Yingying Fan,Dongdong Qin,Li Niu
Photocatalytic synthesis of ammonia (NH 3 ) from nitrogen (N 2 ) offers a promising strategy for carbon neutrality, as it avoids the energy-intensive and carbon-emitting industrial processes. The exploration of high-efficiency N 2 photofixation systems for photocatalytic N 2 reduction reaction (pNRR) is critical but it remains a challenge since the lack of rational structural design and atomic-level insights into molecular N 2 activation mechanism. Herein, an atomically dispersed single-atom palladium (Pd) active sites decorated oxygen-deficient molybdenum oxide (Pd/MoO 3-x ) was creatively designed for assessing pNRR performance. Interestingly, the integration of single-atom Pd active sites in MoO 3-x can significantly weaken the N≡N bond of adsorbed N 2 and effectively lower the activation energy barrier during the pNRR process. This is attributed to the fact that the modified Pd single-atom sites of Pd/MoO 3-x play a dominant role in the N 2 spontaneous adsorption process as well as possess a remarkable photogenerated electron trapping ability, which could be assisted to inject electrons into N 2 antibonding orbital, thus significantly accelerates the reaction kinetics. Consequently, the Pd/MoO 3-x photocatalyst reaches an impressive NH 3 yield rate of 103.2 μgg cat . −1 h −1 , which is superior to that of pristine MoO 3-x (21.2 μgg cat . −1 h −1 ) and commercial MoO 3 (6.5 μgg cat . −1 h −1 ), respectively. The present study not only creates a reliable approach to expand efficient N 2 photofixation system under mild conditions through the fabrication of atomically dispersed monometallic active sites, but also offers atomic-level insights into the underlying mechanism of pNRR catalytic process.
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高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
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2024
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IF 8
Xiang Lu,Yuan Qu,Feiyu Zhang,Ziwen Ding,Haotian Zheng,Yuhua Lei,Song Liu,Siqi Li
Designing sensing materials with effective porous structure and compositions is a crucial strategy for constructing high-performance gas-sensitive devices. Herein, a dodecahedral mesoporous carbon derived from metal-organic frameworks (CMOF), e.g. Zeolitic Imidazolate Framework-8 (ZIF-8) derived porous carbon (ZIF-8-C) was prepared, and subsequently, three-dimensional (3D) hollow dodecahedral ZIF-derived carbon-polyaniline (PANI) based (ZCPx, x representing the mass fraction of ZIF-derived carbon) hierarchical hybrid materials were constructed by introducing protonated polyaniline on the surface of MOF carbon via in-situ oxidative polymerization. The MOF-derived structure provides a substantial interface surface area for the hybrid material, enabling rapid adsorption and charge transfer, along with essential structural stability. The 3D hollow ZCP50 hybrid material prepared exhibits a wide detection range (0.1–500 ppm), repeatability, acceptable long-term stability, and an 8.3 times response enhancement versus PANI. The above performance is attributed to the significant synergistic effect between ZIF-8-C and PANI. The unique design of this 3D framework holds promising potential for the commercial application of room-temperature gas sensors.
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高影响因子
Engineering
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2025
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IF 11.6
Ying Zhu,Jingjing Liu,Guangzhi He,Shaohua Xie,Wenpo Shan,Zhihua Lian,Fudong Liu,Hong He
Catalytic activity and hydrothermal stability are both crucial for the application of the selective catalytic reduction of NO x with NH 3 (NH 3 -SCR catalyst) in diesel vehicles. In this study, a tin (Sn)-modified Ce–Nb mixed-oxide catalyst was synthesized as an NH 3 -SCR catalyst for NO x emission control. After the introduction of Sn, both the NH 3 -SCR activity and the hydrothermal stability of the catalyst were remarkably promoted. Even after hydrothermal aging at 1000 °C, the developed Ce 1 Sn 2 Nb 1 O x catalyst achieved more than 90% NO x conversion at 325–500 °C. Various methods, including N 2 -physisorption, X-ray diffraction, in-situ high-temperature X-ray diffraction, high-resolution transmission electron microscopy, X-ray photoelectron spectroscopy, X-ray absorption fine-structure spectroscopy, temperature-programmed reduction of hydrogen, temperature-programmed desorption of ammonia, and density functional theory calculations were used to investigate the promotional effects induced by the Sn species. The characterization results showed that the addition of Sn not only promoted the formation of the Ce–Nb active phase but also improved its thermal stability, contributing to the excellent NH 3 -SCR performance and hydrothermal stability. This study provides an excellent sintering-resistance catalyst for the application of diesel engine NO x emission control.
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高影响因子
RESEARCH ON CHEMICAL INTERMEDIATES
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2025
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IF 3.5
Li Xinyu,Li Jingqi,Li Na
This study investigated the effects of sequential acid treatment and phosphorus incorporation on the performance of Fe–Mn-Ce composite metal oxide catalysts. The FeMnCeO x catalyst was prepared using the sol–gel method and modified through two methods: treatment with phosphoric acid alone and a sequential treatment with phosphoric acid followed by sulfuric acid. The results show that the sequentially acid-treated catalyst exhibited over 90% NO x conversion and N 2 selectivity in the temperature range of 200–350 °C, outperforming other catalysts. Characterization analyses such as XRD and NH 3 -TPD revealed that acid modification enhanced the surface acidity and redox properties of catalysts. XPS analysis showed that sequential acid treatment increased the surface chemisorbed oxygen content of the catalyst and optimized its surface structure. In-situ DRIFTS spectroscopy further elucidated that the catalytic reaction follows both Langmuir–Hinshelwood and Eley–Rideal mechanisms concurrently.
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高影响因子
ENVIRONMENTAL RESEARCH
·
2025
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IF 7.7
Bo Song,Zhenxing Shen,Qingzhu Tian,Guiling Zhou,Qin Peng,Hao Fan,Jia Liu
Volcanic rock is a natural mineral with a porous structure and rich in various metal oxides. It has been used in environmental applications such as water and soil pollution remediation as stable chemical properties and low cost. In this work, volcanic rock was used in the field of nitrogen oxide control, and the feasibility of preparing NH 3 - Selective Catalytic Reduction catalyst was evaluated. The catalyst AVR-10Mn-450 was prepared by acidification-impregnation-calcination process, and it can achieve more than 90 % denitration effect at 175 °C, 25000 h −1 . It removes nitrogen oxides through the Eley–Rideal and Langmuir–Hinshelwood pathways. AVR-10Mn-450 has the advantages of simple preparation and low cost compared with the mainstream nano-denitration catalysts. It can be applied to the pretreatment of industrial flue gas such as cement plant or glass plant, thereby extending the service life of the precious metal or nano-catalyst at the back end. This work not only realizes the high-value resource utilization of volcanic rock, but also reduces the production cost of denitration catalyst.
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PubMed
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2025
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IF 7.7
Xinru Zhang,Yijie Wang,Lei Zhang,Xiaohai Zhang,Bao Hao,Xiaorui Liang,Helei Dong,Yongqiang Qin,Qiulin Tan
The real-time and accurate detection of ammonia is critical for food freshness testing, agricultural monitoring, and respiratory health diagnostics. Recently, flexible gas sensors have garnered attention owing to their potential for integration into smart wearable electronics and display devices. However, the development of high-performance, low-power, and stable devices remains challenging. In this study, a chemoresistive sensor based on poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS)/MXene composites is designed, wherein the application of a genetic algorithm-optimized back propagation neural network to compensate for humidity leads to a significantly enhanced detection accuracy. Notably, the use of a genetic algorithm-optimized back propagation neural network reduces the detection error from 8.06 % to 1.3 % in the presence of 50 ppm NH 3 . A wireless Bluetooth monitoring system is integrated to enable real-time data transmission and remote monitoring. This sensor detects ammonia within the range of 0.6–1000 ppm, demonstrating an excellent stability, selectivity, and flexibility, thereby confirming the synergistic effects between PEDOT:PSS and MXene. Importantly, in application tests, the developed system reliably assesses meat spoilage and farm ventilation levels, indicating its high applicability and reliability. Successful human breath tests also open new possibilities for the application of this sensor in respiratory health monitoring. Ultimately, this study offers a convenient and efficient approach for food quality assurance, disease diagnosis, and environmental monitoring.
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