Molecular Catalysis
·
2025
·
IF 4.9
Lei Xia,Fang-Jing Liu,Meng-Jie Wang,Han-Bing Zhang,Jing Zhang,Yao Lu,Le-Le Qiu,Xian-Yong Wei,Yun-Peng Zhao
Production of cyclohexanone through selective hydrogenation of phenol under mild conditions has attracted much attention. Herein, a NaOH-modified Pd/WO 3 rich in oxygen vacancies for selective hydrogenation of phenol was prepared through impregnation method. The highest catalytic activity was exhibited on NaOH-Pd/WO 3 with 25 wt % addition of NaOH, and phenol achieved 100 % conversion at 90 °C and 0.7 MPa H 2 for 2 h, with a cyclohexanone selectivity of 95.3 %. The turnover frequency (TOF) of NaOH-Pd/WO 3 is approximately 3.5 times higher than that of the Pd/WO 3 . Detailed catalyst characterization and theoretical calculations reveal that the high activity and selectivity of NaOH-Pd/WO 3 for phenol hydrogenation to cyclohexanone are highly correlated with the concentration of oxygen vacancies in the catalyst. In-situ infrared and Raman analyses reveal that the OH - introduced by NaOH reacted with the lattice oxygen in WO 3 to abstract oxygen from the lattice, generating a significant number of oxygen vacancies. The possible reaction mechanisms for phenol hydrogenation were elucidated through combined density functional theory calculations and isotopic labeling experiments. This strategy of improving catalytic activity and selectivity by regulating the concentration of oxygen vacancies provides a theoretical basis for the design and optimization of industrial catalysts.
研究领域:
催化
·
化学工程
·
材料科学
·
物理化学
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DOI
高影响因子
JOURNAL OF CATALYSIS
·
2024
·
IF 6.5
Wei Jia,Wengang Liu,Yuandong Cui,Hang Song,Chengfeng Zhou,Wei Jiang,Haoxi Ben,Xiaoli Yang,De Chen
Converting cellulose into C 2 alcohols presents a sustainable alternative to fossil fuels, contributing to the development of eco-friendly and economically viable biofuels and chemicals. Tungsten oxide (WO 3 ) is a key solid acid catalyst for this process, yet limited research explores its diverse morphologies and unique catalytic effects. This study investigates diverse WO 3 morphologies (nanosheets, nanoflowers, nanoblocks, and tetrahedral octahedra) in combination with Pd for converting cellulose to C 2 alcohols. Optimized conditions with Pd/o-WO 3 catalyst resulted in the highest C 2 alcohols (ethylene glycol and ethanol, 80.9 %), notably yielding 64.8 % ethylene glycol. Extensive characterizations and DFT calculations reveal the smaller element occupancy rates and a longer W-O bond length led to a large number of crystal defects over Pd/o-WO 3 . It facilitated the formation of W 5+ –OH sites and Pd-O(H)-W interactions, further synergistically enhancing hydrogenation ability and acidity. Designed experiments to elucidate cellulose conversion pathways, including hydrolysis, retro -aldol condensation, and hydrogenation. This study emphasizes the unique impact of WO 3 morphologies and underscores the importance of supporting crystal defects for catalytic performance in eco-friendly biofuel and chemical production.
研究领域:
催化化学
·
可再生资源与环境科学
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产品关联
DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2024
·
IF 8
Xuan-Yu Yang,Hao-Nan Chen,Li-Juan Yue,Fei-Long Gong,Ke-Feng Xie,Shi-Zhong Wei,Yong-Hui Zhang
The design of novel functional nanostructures for advanced chemical engineering field is of great importance. In this work, Pd-modified Na-doped WO 3 nanorods are rationally designed for rapid and detection of hydrogen, which is a green and clean energy in modern industry. Notably, and H + as well as citrate ions play an important role in the formation of 1D nanorods, and the morphology formation mechanism is explored. Here, inspired by the novel Pd-modified Na-doped WO 3 nanorods structure, the Pd-400-Na/WO 3 NRs exhibit high sensing ability with ultra-high response to hydrogen (R a /R g = 218@25 ppm) and fast response time (3 s). The combination of experimental and theoretical results shows that Na doping effectively modulates the d-band center of Pd and enhances activation and desorption of H 2 on the Pd surface. The 1D porous structure also facilitates the diffusion of H 2 within the framework, and accelerate the charge transformation. Meanwhile, the surface Pd 0 sites are assigned as the surface active sites for H 2 adsorption and activation, and Pd 2+ sites facilitate the desorption process. Our work paves the new insights for the design of high performance H 2 sensing materials.
研究领域:
材料科学
·
化学工程
·
纳米技术
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DOI
高影响因子
ACS Catalysis
·
2026
·
IF 13.1
Can Cheng,Yaolin Wang,Jia-nan Wang,Haomiao Xu,Wenjun Huang,Zhisong Liu,Wei Li,Yuyang Li,Zan Qu,Xin Tu,Naiqiang Yan
Plasma-catalytic CO2 hydrogenation to CO offers a promising route for carbon-neutral chemical synthesis. However, its advancement is constrained by low energy efficiency and limited mechanistic insight. Here, we developed an oxygen vacancy-engineered Pd-WO3–x catalyst supported on nickel foam (NF), which exhibits enhanced performance in ambient plasma-driven CO2 conversion. The system leverages the conductive properties of NF to spatially divide the discharge zone into streamer and filamentary discharge zones, thereby enhancing plasma activation and interfacial charge transfer. Catalyst characterization reveals that Pd plays a critical role in stabilizing metastable oxygen vacancies (OVs) within WO3–x, which function as electron reservoirs to promote CO2 dissociation into CO. Density functional theory calculations and in situ spectroscopic studies confirm that Pd facilitates H2 dissociation, while vibrationally excited CO2 generated in the plasma gas phase preferentially adsorbs at OV sites. At a specific energy input of 33.6 kJ L–1, the system demonstrates superior performance, achieving 54.9% CO2 conversion with 99.8% selectivity toward CO, surpassing typical plasma-catalytic benchmarks. The catalyst exhibited good stability over 100 h of continuous operation, with a slight decrease in CO2 conversion (<10%) and nearly unchanged CO selectivity (>99%) due to strong metal–support interactions and the conductive nature of NF. This work demonstrates that OV engineering provides a promising strategy for designing efficient plasma-catalytic systems for CO2 conversion.
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DOI
PubMed
高影响因子
ACS Nano
·
2026
·
IF 17.3
Ruofan Zhang,Xingxing Xie,Zanhong Deng,Jie Meng,Xiaohua Ji,Qi Zhang,Ruoqing Zhang,Siyuan Liu,Dandan Rong,Shimao Wang,Xiaodong Fang,Gang Meng
Abstract Selective detection of trace (weakly reducing) dimethyl sulfide (DMS) in highly humid exhaled breath using metal oxide semiconductor (MOS) sensors, with the presence of strong reducing H2S interference gas, is essential for the early diagnosis of hepatic diseases. However, it remains a big challenge in principle. Herein, a bilayer MOS sensor with a Pd–WO3 sensing film and a CuO/Al2O3 filtering overlayer was proposed. The temperature-dependent H2S catalytic oxidation experiment suggests that CuO could effectively filter H2S even under room temperature. Dispersing the CuO particles into insulative Al2O3 carrier could not only selectively remove H2S without significant consumption of DMS but also isolate the underlying Pd–WO3 sensing layer’s response signal from interference caused by that of CuO. By adding the CuO/Al2O3 1:9 filtering overlayer, the response ratio of DMS to H2S was significantly enhanced from 3.3 to 50.4, furthermore, an ultrahigh response (701.3) to 10 ppm DMS, and a low limit of detection of 10 ppb under 90% RH were achieved, which promises the future breath disease diagnosis.
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Xiangdong Cao,Jihua Tang,Chenchen Xu,Jiaqi Wang,Youfu Geng,Duo Yi,Xuejin Li,Yu Du,Xiaoqing Tian
Triethylamine (TEA) is a kind of flammable and pungent gas, which extensively exists in our daily life. It is paramount important to monitor ppb-level TEA rapidly and selectively at low temperatures. Herein, tungsten oxide hollow microspheres were successfully co-modified by different amount of Pd and N719, and were used to construct semiconductor gas sensor. TEA sensing properties were tested for the N719-Pd/WO 3 and Pd/WO 3 composites under various light illumination conditions. It is exciting to observe that the 0.3 wt% N719-Pd/WO 3 sensor exhibits excellent TEA detectability in terms of ultra-high response (1410, 50 ppm), low operating temperature (100 °C), fast response speed (25 s) and low detection limit (27 ppb) under white light illumination, which are superior to WO 3 sensors loaded with other Pd and N719 concentration as well as upon other light illumination conditions. This excellent sensing performance indicates that the proposed dual-effect improved sensitization by combining noble metal functionalization with visible light excitation offers an effective design for highly sensitive and efficient gas sensors based on wide-band gap semiconductors.
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产品关联
DOI
高影响因子
ACS Sensors
·
2026
·
IF 10.9
He-Jie Wang,Hao-Nan Chen,Xuan-Yu Yang,Fei-Long Gong,Ke-Feng Xie,Shi-Zhong Wei,Yong-Hui Zhang
The development of highly sensitive and reliable hydrogen detection technology is a critical prerequisite for the safe and large-scale application of green hydrogen energy. Pd-based metal oxide semiconductor sensors exhibit decent sensing performance; however, their development for hydrogen detection is hindered by competitive adsorption of hydrogen and oxygen on the surface and sluggish reaction kinetics due to limited active interfaces. Here, a series of Pd nanoparticle-decorated, K+ interstitial doping WO3 nanosheets (PdNP-K/WO3-x) were synthesized. The optimized PdNP-K/WO3-15 sample exhibited exceptional H2 sensing performance, including a high response (Ra/Rg = 1235.94 to 50 ppm H2) at a low temperature of 130 °C, with fast response/recovery. This enhancement stems from synergistic effects where K+ interstitial doping increases electron density and oxygen vacancies in WO3, improving charge transfer and strengthening the W-O-Pd interface. The resulting electron-rich environment also shifts the d-band center of Pd, enhancing hydrogen desorption and spillover, while reducing competitive oxygen adsorption to free up more Pd active sites. The material also showed promising room-temperature sensing, indicating strong application potential and providing a theoretical basis for designing high-performance alkali metal ion-doped metal oxide materials.
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产品关联
DOI
PubMed
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2020
·
IF 7.1
Yun-Zhi Dai,Shu-Yu Liang,Chao Lv,Gong Wang,Hong Xia,Tong Zhang,Hong-Bo Sun
Micro/nanoscale gas sensors attracted more attention because of their potential application in the emerging areas such as electronic capsules, wearable devices, and microdrone detectors. However, it is still a challenge to achieve micro/nanoscale sensors with controllable processing parameters of active components and fast response and recovery capability. Here, a flexible and high precision femtosecond laser direct-writing technology is selected to print various semiconductor metal oxides nanoparticles into microscale designable patterns with mask-free. And by using Pd-doped WO 3 • x H 2 O nanoparticles we have fabricated single Pd-WO 3 • x H 2 O microwire (SPWM) as gas sensors, which represented high sensitivity, faster response and recovery. Especially, for ammonia gas sensing the SPWM with pre-designed lengths can possess ultrafast response with response/recovery time of 1.4/3.3 s in 50 ppm NH 3 , or low limit-of-detection of 1 ppm at room temperature. This kind of micro-scale gas sensor is expected to be applied to human health monitoring, environmental air detection and other integrated intelligent devices.
研究领域:
材料科学
·
传感器技术
·
纳米技术
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产品关联
DOI
高影响因子
Nature Communications
·
2023
·Vol. 14
·期 1
·1-10
·
IF 16.6
Zhang Wenqing,Xi Dawei,Chen Yihong,Chen Aobo,Jiang Yawen,Liu Hengjie,Zhou Zeyu,Zhang Hui,Liu Zhi,Long Ran,Xiong Yujie
Oxidative carbonylation of methane is an appealing approach to the synthesis of acetic acid but is limited by the demand for additional reagents. Here, we report a direct synthesis of CH 3 COOH solely from CH 4 via photochemical conversion without additional reagents. This is made possible through the construction of the PdO/Pd–WO 3 heterointerface nanocomposite containing active sites for CH 4 activation and C–C coupling. In situ characterizations reveal that CH 4 is dissociated into methyl groups on Pd sites while oxygen from PdO is the responsible for carbonyl formation. The cascade reaction between the methyl and carbonyl groups generates an acetyl precursor which is subsequently converted to CH 3 COOH. Remarkably, a production rate of 1.5 mmol g Pd –1 h –1 and selectivity of 91.6% toward CH 3 COOH is achieved in a photochemical flow reactor. This work provides insights into intermediate control via material design, and opens an avenue to conversion of CH 4 to oxygenates.
研究领域:
化学工程
·
光化学
·
材料科学
·
催化
✓ 已验证
产品关联
DOI
PubMed
高影响因子
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