FUEL
·
2024
·
IF 6.7
Jianfei Luo,Langlang Wang,Yibing Xie,Ping Ning,Yiran Xiong,Hang Zhang,Yixing Ma,Shao Zhang,Xueqian Wang
Existing processes for transforming arsine (AsH 3 ) into toxic arsenic oxides (As x O y ) through catalytic oxidation do not meet economic requirements. In contrast, the catalytic decomposition method stands out due to its ability to both remove AsH 3 and obtain elemental arsenic (As 0 ) as a valuable product. A series of blank molecular sieves (HZSM-5, 13X, MCM-41, and TS-1) was applied to the catalytic decomposition performance of AsH 3 . At a catalytic decomposition temperature of 100 ℃, the HZSM-5 zeolite exhibited exceptional performance, achieving a D 90% value (the duration for which the AsH 3 removal efficiency remained above 90 %) exceeding 40 h. Moreover, up to 83.1 % of the product was As 0 . Comprehensive characterization revealed that the surface of the HZSM-5 zeolite contained a large number of strong acid sites, which played a key role in As 0 generation. In situ diffuse reflectance infrared spectroscopy further revealed the activation behavior of O 2 at the Brønsted acid sites on HZSM-5. To assess its suitability in industrial applications, the AsH 3 removal performance of the HZSM-5 molecular sieve was investigated in the presence of actual gas components (CO, H 2 S, PH 3 ). This study provides new ideas for the effective catalytic decomposition of AsH 3 and the recovery of valuable products in industry.
CAS / MDL:
研究领域:
环境科学
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催化化学
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2020
·
IF 7.489
Yaoyu Zhang,Yuxing Wang,Yue Liu,Qingji Ying,Zhongbiao Wu
A sequence of CuCeO x -HZSM-5 composite catalysts at different Cu-Ce loading synthesized by the citric acid complex impregnation method were evaluated for the catalytic oxidation of acetonitrile. Among which, the 2CuCeO x -HZSM-5 sample exhibited the best degradation efficiency. In the temperature range of 225–350 °C, its activity and mineralization rate were approximately 100%, and the N 2 selectivity remained more than 93%. The characterization results revealed that all the samples showed an existence of isolated Cu 2+ species. And more Cu-Ce mixed oxides covered on HZSM-5 at an elevated Cu-Ce content, leading to the enhanced reducibility. In situ DRIFTS results showed that both oxidation and hydrolysis reaction routes proceeded during the degradation of acetonitrile over the composite catalysts. Their synergism was crucial to guarantee both high activity and N 2 selectivity. The highly dispersed CuO x species ensured the superior activity of the 2CuCeO x -HZSM-5 sample. And Cu 2+ exchanged HZSM-5 zeolite would be beneficial to N 2 selectivity owing to the improved internal SCR (Selective Catalytic Reduction) reaction to reduce NO x from oxidation routes. Additionally, the mineralization rate was lowered with the formation of carbonaceous products like CH 4 and CO for the catalysts at low Cu-Ce loading due to the lack of redox capacity.
研究领域:
催化
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环境科学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Yihua Yue,Jian Tian,Jiechao Ma,Shui Yang,Wen Li,Jiale Huang,Qingbiao Li,Guowu Zhan
Herein, Ga-ZnZrO x &ZSM-5 bifunctional catalysts were designed for CO 2 thermal hydrogenation to aromatics, particularly, aiming to enhance the selectivity of high-value BTX ( i.e. , benzene, toluene, and xylene). It was evident that the exterior surface properties and acidity of ZSM-5 can be effectively tailored by in-situ silicon deposition originating from the rice husk template. Catalytic performance assessments demonstrate an optimized catalyst achieving 88.1 % aromatics selectivity (exclusive CO) in a single pass, with a notable 45.2 % BTX selectivity within total aromatics and a low CO selectivity of 23.6 %. This superior performance is attributed to the in-situ silicon deposition on ZSM-5 during one-pot synthesis and the optimized spacing between Ga-ZnZrO x and ZSM-5 facilitated by the rice husk platform. Furthermore, in-situ DRIFTS analysis identifies key reaction intermediates. This study offers an effective strategy for tuning zeolite acidity using rice husks, while modulating metal oxide-zeolite proximity on the bio-SiO 2 platform, thus boosting CO 2 conversion to aromatics.
研究领域:
催化
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化学工程
·
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2020
·
IF 9.038
Hao Lu,Xinlei Yao,Jing Li,Shuiliang Yao,Zuliang Wu,Huanhuan Zhang,Hanghao Lin,Tomohiro Nozaki
Plasma-catalytic oxidation of particulate matter (PM) has potential applications for diesel exhaust cleaning. There is a grand requirement to explore the mechanism of carbonaceous PM oxidation for the development of plasma catalysts. Herein, Au/γ-Al 2 O 3 was used to catalyze the gasification of the graphitic carbon. A modified diffuse reflectance infrared Fourier transform spectrometer equipped with a mass spectrometer was originally utilized to in situ characterize the surface intermediates of graphite on Au/γ-Al 2 O 3 and the gaseous products during the discharges processes in the O 2 -He balanced gases. It was found that O atoms and O 3 play important roles in the formation of surface oxygen complexes (SOCs) and facilitate the gasification of SOCs to CO 2 in the presence of Au/γ-Al 2 O 3 . The findings are helpful to understand the plasma-catalytic oxidation mechanism of PM and further develop efficient plasma catalysts.
研究领域:
环境科学
·
催化化学
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Kejing Wang,Yongjun Liu,Zhiwen Li,Nan Cui,Lei Sun,Wei Huang
The valence states of Cu site are regarded as an important factor affecting the performance of syngas to higher alcohols (C 2+ OH). Regrettably, the role of Cu 0 and Cu + in CO hydrogenation to higher alcohols remains controversial due to the complexity of the reaction. In this study, Cu 0 and Cu 2 O powders are directly added as the precursors to adjust the ratios of Cu + /(Cu 0 +Cu + ) and Cu particle sizes in CuZnAl catalysts by a complete liquid-phase (CLP) technology. The CAT-Cu 0 catalyst with higher Cu 0 content shows the highest CO conversion (>15%) ascribing to the biggest S Cu , but is also accompanied by the highest CO 2 selectivity (>40%), while the CAT-Cu + catalysts with higher Cu + content displays relative better C 2+ OH selectivity (>60%) and stability due to a higher probability of CO insertion. In-situ DRIFTS experiments reveal that a synergy between larger Cu particle sizes (30～40 nm) and surface Cu + sites, in which larger Cu sizes enhances the probability of bridge CO adsorption, thereby favoring the C–O bond dissociation for CH x formation. Meanwhile, Cu + active sites provide a higher probability for CO/CHO insertion to form CH 3 CHO*/CH 2 CO* intermediates. This study further deepens our understanding of the critical controlling factors for highly selective synthesis of C 2+ OH from syngas over Cu-based catalysts.
研究领域:
化学工程
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催化
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF THE ENERGY INSTITUTE
·
2024
·
IF 5.6
Xueyu Zan,Shiqi Tao,Chaoyu Zhang,Yixiao Wu,Yongjun Liu,Wei Huang
Direct conversion of methane and carbon dioxide into acetic acid is a dream way to address the two greenhouse gases, but is challenged by their chemical inertness. Cu and Pd are promising candidates both in CH 4 and CO 2 activation as well as the subsequent C-C coupling reactions at low temperature. Herein, we report that acetic acid can be produced by the direct coupling of CH 4 and CO 2 in the presence of H 2 O 2 over Cu-Pd/Al 2 O 3 catalysts at 50 °C. Results show that the acetic acid yield reaches 48.1 μmol·g cat −1 ·h −1 on the optimized reaction condition over Cu 3.8 -Pd 1.6 /Al 2 O 3 catalyst, which is higher than that of either mono-Cu or mono-Pd catalyst. Extensive characterization indicates the higher activity of Cu 3.8 -Pd 1.6 /Al 2 O 3 catalyst is attributed to the strong synergistic effect between Cu and Pd, which results in the formation of CuPdO 2 phase, and thus promoting the electron transfer from Cu to Pd. DRIFTS experiments reveal that acetic acid is produced by the coupling of CH 3 * and COOH* over CuPdO 2 active sites via Langmuir-Hinshelwood mechanism, where CH 3 * is originated from CH 4 dehydrogenation step, and COOH* may formed by the activation of CO 2 by H 2 O 2 . This study provides a new approach for the co-conversion of CH 4 and CO 2 into acetic acid at low temperature.
研究领域:
化学工程
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催化
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
MOLECULES
·
2024
·Vol. 29
·期 10
·2255
·
IF 4.2
Yan Cui,Zequan Zeng,Yaqin Hou,Shuang Ma,Wenzhong Shen,Zhanggen Huang
Noble metals have become a research hotspot for the oxidation of light alkanes due to their low ignition temperature and easy activation of C-H; however, sintering and a high price limit their industrial applications. The preparation of effective and low-noble-metal catalysts still presents profound challenges. Herein, we describe how a Ru@CoMn2O4spinel catalyst was synthesized via Ru in situ doping to promote the activity of propane oxidation. Ru@CoMn2O4exhibited much higher catalytic activity than CoMn2O4, achieving 90% propane conversion at 217 °C. H2-TPR, O2-TPD, and XPS were used to evaluate the catalyst adsorption/lattice oxygen activity and the adsorption and catalytic oxidation capacity of propane. It could be concluded that Ru promoted synergistic interactions between cobalt and manganese, leading to electron transfer from the highly electronegative Ru to Co2+and Mn3+. Compared with CoMn2O4, 0.1% Ru@CoMn2O4, with a higher quantity of lattice oxygen and oxygen mobility, possessed a stronger capability of reducibility, which was the main reason for the significant increase in the activity of Ru@CoMn2O4. In addition, intermediates of the reaction between adsorbed propane and lattice oxygen on the catalyst were monitored by in situ DRIFTS. This work highlights a new strategy for the design of a low-noble-metal catalyst for the efficient oxidation of propane.
研究领域:
催化
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化学工程
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
BIORESOURCE TECHNOLOGY
·
2025
·
IF 9
Jirong Long,Yuxuan Mao,Yiwei Long,Guozhang Chang,Lungang Chen,Wenguang Zhou,Jinxing Long,Yong Liu
Hydrodeoxygenation of lignin-derived phenols into high-value cycloalkanes under mild conditions is challenging. Herein, we report a Ru NPs @HZSM-5 catalyst with a unique metal-support interactions that achieves 100 % guaiacol conversion and 99.7 % cyclohexane selectivity at 160 °C and 1 MPa H 2 . Comparative studies with single-atom and aggregated Ru catalysts reveal that well-dispersed Ru nanoparticles coupled with acid sites offer superior activity and selectivity. Kinetic analysis and in situ DRIFTS demonstrate a sequential mechanism involving rapid hydrogenation of the aromatic ring followed by rate-limiting deoxygenation steps. Characterizations and CO-DRIFTS confirm particle sizes, optimal metal-support interactions, and enhanced acidity in Ru NPs @HZSM-5. Theoretical calculations further reveal favorable electronic states and lower energy barriers for deoxygenation on Ru NPs @HZSM-5. The catalyst also shows broad substrate compatibility, efficiently converting various lignin-derived phenolics. This work provides valuable insights into the critical synergy between metal nanoparticles and acidic supports for efficient lignin upgrading.
研究领域:
催化
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可再生能源
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生物质转化
·
多相催化
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可持续化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Jiahe Zhai,Hui Wang,Abdelkader Labidi,Long Zeng,Yu Huang,Chuanyi Wang
Removing low-concentration NO in the air by means of photocatalytic technology is a promising approach. Herein, our work pins down the mechanism of cobalt metal doping within the lattice of Bi 4 Ti 3 O 12 (BTO) for the photocatalytic NO conversion. As a result, the Co-BTO exhibits a NO conversion efficiency of 58.3 %, which is substantially higher than that of BTO (30 %). More interestingly, the Co-BTO also shows a lower production of intermediate NO 2 than that of the BTO. These findings demonstrate that within Co-BTO, both Co²⁺ and Co³ ⁺ coexist. The redox cycle between these two cobalt species engenders active sites possessing strong reducing capabilities for O₂ which can be adsorbed and activated at the Co sites, thereby generating superoxide radicals (•O₂⁻). Furthermore, the doping of a certain portion of cobalt broadened light absorption and enhanced the separation efficiency of photogenerated carriers, further facilitating the activation of O₂. Lastly, electron spin resonance (ESR) and in-situ diffuse reflective infrared Fourier transform spectroscopy (in-situ DRIFTS) were respectively utilized to further clarify the active species involved in the photocatalytic oxidation of NO and its adsorption and conversion pathways from a mechanistic standpoint. Overall, this work represents a novel endeavor for the advancement of visible-light-driven photocatalysts usage for environmental remediation against NO pollution.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Catalysis Science & Technology
·
2016
·Vol. 6
·期 24
·8516-8524
·
IF 5.287
Lei Huang,Kaiwen Zha,Supawadee Namuangruk,Anchalee Junkaew,Xin Zhao,Hongrui Li,Liyi Shi,Dengsong Zhang
Surface engineering of TiO2 is significant in the SCR reaction and worth studying. In a previous study, we found that TiO2 nanosheets (TiO2-NS) with the (001) plane exhibited a much better SCR performance than TiO2 nanoparticles (TiO2-NP) with the (101) plane. In this work, in situ DRIFTS and DFT calculations were applied to address the promotional effect of the (001) plane of TiO2-NS in the SCR reaction. The behavior of adsorption and desorption of NOx and NH3 on the two surfaces was studied. It was found that NH3 adsorbed on both TiO2-NS and TiO2-NP was in the form of NH3(g) on the Lewis acid sites. NOx on TiO2-NP were mainly trans-(NO)2 and N2O4 which were non-reactive. Differently, NO on TiO2-NS was mainly in the form of NO2 which was probably due to the high energy and abundant active oxygen species of the (001) facet. The formed NO2 could trigger the subsequent ‘fast SCR’ reaction thereafter promoting the activity. Therefore, TiO2-NS with more (001) facets had better SCR activity than TiO2-NP with the exposed (101) facet.
研究领域:
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Mingrui Geng,Zhizhen Wang,Denghui Wang
Formaldehyde (HCHO), a ubiquitous indoor organic pollutant, severely threatens human health. Developing efficient and low-energy catalytic materials for room-temperature HCHO purification remains an urgent priority. In this work, Fe y MnO x catalysts were synthesized via a facile coprecipitation method. The Fe doping effectively modulated the morphology and crystallinity of δ-MnO 2 while inducing the formation of surface oxygen vacancies, thereby enhancing the capability to generate surface reactive oxygen species. Under a gas hourly space velocity (GHSV) of 150 L·g cat –1 ·h –1 , the catalyst achieved > 99 % removal efficiency for 100 ppm HCHO, along with exceptional stability. In situ DRIFTS reveals the influence of Fe doping on the catalytic reaction pathway for HCHO. This work demonstrates that the Fe doping strategy successfully optimizes the microstructure and surface chemical properties of δ-MnO 2 , resulting in outstanding room-temperature HCHO removal performance, providing valuable insights into defect engineering for optimizing transition metal oxide catalysts.
研究领域:
环境催化
·
材料科学
·
室内空气净化
·
过渡金属氧化物
·
缺陷工程
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Guang-Rong Ding,Yao-Feng Wang,Guo-Yi Duan,You-Qian Fan,Bao-Hua Xu
In this study, a tungstated zirconia (WOx/ZrO2) catalyst was developed for the continuous synthesis of adiponitrile (ADN) by gas-phase nitrilation of dimethyl adipate (DMA) with NH3. The highest TOFADN could be reached on WOx/ZrO2 bearing ∼1D WOx species (highly dispersed and discontinuous status) at the surface, which, however, delivered the poorest selectivity toward nitrilation (SADN+MCP). In comparison, both efficient and selective transformation of DMA to ADN was achieved by fabricating WOx/ZrO2 with continuously distributed oligomeric WOx species (∼2D) at the surface, either by varying the dosage of the W-reagent in the preparation of WOx(m)/ZrO2 or by doping a proper amount of the Mn element into WOx(5.0)/ZrO2, bearing WO3 NPs. Furthermore, the in situ diffuse reflectance infrared Fourier transform spectroscopy investigations of both independent and competitive adsorptions of ester functionality and NH3 over W–O–Zr, W–O–W, and Zr–O–Zr boundaries at the surface clarified the synergistic effect of these species in the activation of DMA/NH3 and thereby nitrilation.
研究领域:
催化
·
化学工程
·
表面科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）