JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Lijun Yue,Wanjun Zhao,Jinfang Li,Ruifang Wu,Yongzhao Wang,Hongxi Zhang,Yongxiang Zhao
The impact of Indium (In) doping upon the catalytic performance of Pd-Cu/Al 2 O 3 for carbon monoxide preferential oxidation (CO-PROX) in hydrogen (H 2 ) rich atmosphere at low temperature has been studied. A series of catalysts with extremely low palladium (Pd) loading (0.06 wt%) are synthesized by the facile co-impregnation method. When the In/copper (Cu) atomic ratio equals 0.25, Pd-Cu-In 0.25 /Al 2 O 3 can keep 40% CO conversion and 100% carbon dioxide (CO 2 ) selectivity at least 120 min at 30 °C, which is significantly superior to the catalytic performance of Pd-Cu/Al 2 O 3 . The elaborate characterization findings reveal that the added In species to Pd-Cu/Al 2 O 3 causes Indium oxide (In 2 O 3 ) to generate, which produces the interaction of In 2 O 3 with Pd-Cu/Al 2 O 3 , further promoting the dispersion of copper chloride hydroxide (Cu 2 Cl(OH) 3 ). Moreover, the modification of In facilitates the re-oxidation of Pd 0 to Pd + through reducing the formation of palladium hydride (PdH x ) during the CO-PROX reaction. Meanwhile, the addition of In leads to the decrease of Cu + electron cloud density, making it easier to be oxidized to Cu 2+ . Collectively, the easy re-oxidation of Pd 0 and Cu + is favorable to fulfill the Wacker cycle between Pd and Cu species, thus improving the catalytic performance for CO-PROX.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Wenjun Yan,Yun Liu,Yan Bai,Yulong Chen,Houpan Zhou,Waqar Ahmad
In this paper, we present the design and evaluation of an intelligent MEMS sensor employing the oxidized medium-entropy alloy (O-MEA) of FeCoNi as the gas-sensing material. Due to the specific catalytic exothermic reaction of the O-MEA on H2/CO, the sensor shows great selectivity for H2 and CO at 150 °C of the integrated microheater in the MEMS device, with the theoretical detection limit of 0.3 ppm for H2 and 0.29 ppm for CO. The MEMS heater, capable of instantaneous temperature changes in pulse operation mode, offers a novel approach for thermal modulation of the sensor, which is crucial for the adsorption and reaction of H2/CO molecules on the sensing layer surface. Consequently, we investigate the gas-sensing capabilities of the sensor under pulse heating modes (PHMs) of the MEMS heater and then propose the gas-sensing mechanism. The results indicate that PHMs significantly not only reduce the operating temperature and power consumption but also enhance the sensor’s functionality by providing multivariable response signals, paving the way for intelligent gas detection. Based on the high selectivity to H2 and CO, transforming the transient sensing curves into two-dimensional images via Gramian Angular Field (GAF) model and subsequent modeling using a convolutional neural network (CNN) algorithm, we have realized efficient and intelligent recognition of H2 and CO. This work provides insight for the development of low-power, high-performance MEMS gas sensors and further intelligence of individual MEMS sensors.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Ning Li,Chao Ma,Dudu Li,Peng Li,Mao Ye,Ziyue Wang,Zhihua Qiao,Chongli Zhong
Mixed matrix membranes (MMMs), combining the advantages of polymer membranes and porous materials, processing the potential to realize large-scale gas separation applications. However, the interfacial defects in MMMs greatly hindered gas separation performance improvement. Therefore, designing an MMM with high loading and good interfacial compatibility remains a critical issue in promoting the application of MMMs. Herein, during in - situ heating process, the melting of liquid ZIF-62 in PBI polymer can largely fill the interfacial defects in MMMs. The microporous transport channels of ZIF-62 glass in MMMs promoted the H 2 diffusion and inhibited the CO 2 and CH 4 diffusion, thus enhancing the H 2 /CO 2 and H 2 /CH 4 separation of MMMs. For mixed gas testing, the 45 wt% ZIF-62 glass/PBI membrane had the maximum H 2 permeability of 459 barrer, and its H 2 /CO 2 and H 2 /CH 4 selectivities were 23 and 57, higher than the gas separation upper bonds. In addition, ZIF-62 glass/PBI membrane exhibited stable separation performance under 1–5 bar pressure. Therefore, the rational combination of MOF glass and polymer matrix could provide promising potential for reducing the interfacial defects of high-loading MMMs, thus enhancing the gas separation performance.
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Wanpeng Zhou,Ruyao Feng,Miaolian Ma,Zhixuan Hu,Tao Yao,Maofeng Zhang
Natural flavonoids, including quercetin, rutin, baicalein and puerarin have been employed for the first time as efficient catalysts in the alcoholysis of NaBH 4 . Among them, quercetin demonstrates optimal catalytic performance for this reaction, achieving an HGR value of 26374 mL H 2 g cat −1 min −1 when 0.2 g NaBH 4 is catalyzed by 50 mg quercetin. The catalytic activity of quercetin is unparalleled for methanolysis of NaBH 4 , particularly at low-temperature; notably, a high HGR value of 1948 mL H 2 g cat −1 min −1 is observed even at −25 °C. Furthermore, the activation energy for the NaBH 4 methanolysis catalyzed by quercetin within a low temperature range of −25 to 25 °C has been calculated to be 17.2 kJ mol −1 . Investigates into the reusability and regeneration of quercetin reveal that over 74 % of its catalytic activity is retained after five consecutive uses; additionally, complete recovery of catalytic activity can be achieved through simple acid treatment. Moreover, kinetic studies indicate that the reaction orders of NaBH 4 methanolysis catalyzed by quercetin obey to first-order kinetics concerning all concentrations: NaBH 4 concentration, catalyst dosage, and methanol content. This study establishes a foundation for practical application involving NaBH 4 in hydrogen production under cold climate conditions typical in Polar Regions or during severe winters at northern latitudes.
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Xiteng Yan,Xiaohan Chen,Runping Ye,Jingwen Tao,Gang Feng,Feiyang Hu,Honglin Hu,Claudia Li,Kang Hui Lim,Tao Wen,Yuan Wang,Xinhao Li,Rongbin Zhang,Sibudjing Kawi
Ammonia (NH 3 ) decomposition is a practical approach to overcome the challenges associated with hydrogen storage and transportation. The choice of catalyst and understanding the catalytic mechanism are key factors in optimizing H 2 production by NH 3 decomposition performance. In this work, a series of alkali metal-doped Fe-based catalysts were synthesized via a solvothermal method, and the formation of Fe x N active phases was systematically investigated. The Fe-based catalysts were pretreated under different atmospheres (H 2 , NH 3 , and N 2 ), followed by comprehensive characterization using BET, XRD, SEM, NH 3 -TPD, XPS, and other techniques. The optimized catalytic activity for NH 3 decomposition was attributed to the formation of Fe x N active phases, and the formation pathway of Fe x N active phases and their catalytic promotion mechanism were further elucidated through XRD, NH 3 -TPD-MS, and XPS analyses. Significantly, catalysts treated with pure NH 3 exhibited an increase in the electron density of Fe species and a decrease in the apparent activation energy. The incorporation of alkali metal doping further amplified this effect, ultimately leading to enhanced hydrogen production performance from NH 3 decomposition. This work underscores the critical function of the Fe x N active phase in facilitating efficient NH 3 decomposition for hydrogen generation, offering invaluable insights into the development of sophisticated alkali metal-doped Fe-based catalysts.
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Hongquan Fu,Jinhua Wang,Juan Zhang,Dan Liu,Hejun Gao,Yunwen Liao,Hao Yu
Though the different exposed crystal facets of cadmium sulfide (CdS) catalysts have been demonstrated to enhance their photocatalytic activity , the mechanism behind H 2 evolution on these diverse facets remains elusive. Here, we synthesized CdS photocatalysts with co-exposed (101) and (002) crystal facets, incorporating S vacancies via a hydrothermal method within the temperature range from 80 to 240 °C. The resulting CdS nanorods exhibited exposed (002) and (101) crystal facets, demonstrating abundant S vacancies, and showcased a notable photocatalytic hydrogen (H 2 ) evolution activity of 467.67 μmol g −1 ·h −1 —approximately 144 times higher than that of CdS nanoparticles . Both experimental results and density functional theory (DFT) calculations showed the significance of co-exposed (101) and (002) crystal facets as self-constructed crystal homojunctions on CdS, facilitating efficient spatial separation of photogenerated charges. Additionally, co-exposed (101) and (002) crystal facets with S vacancies, stemming from the mismatched lattice, were observed to enhance the adsorption of water (H 2 O) molecules. This, in turn, reduced the energy required for H 2 dissociative adsorption , providing thermodynamic advantages. The understanding of the synergistic effect between self-constructed (101) and (002) facet junctions and S vacancies on CdS for boosting photocatalytic H 2 evolution holds promise for expanding the applications of CdS-based materials in various photocatalytic processes.
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2018
·
IF 4.908
Yaqiu Tao,Lulu Tao,Zhigang Pan,Simin Qiu,Xiaodong Shen
Formic acid is a promising hydrogen storage material for its high H 2 capacity, easy transfer and moderate H 2 regeneration conditions. Active carbon supported Mo 2 C with or without Co doping were used as the heterogeneous catalyst in the decomposition of a high concentrated aqueous solution of formic acid up to 50% on a fixed bed reactor. For a given flow rate and reaction temperature, though higher volume of H 2 is produced per unit time, the increase in formic acid’s concentration reduces both H 2 selectivity and formic acid conversion rate. At 250 °C, a stream of 236 mL/min H 2 was generated continuously at a high H 2 selectivity (91%) and formic acid conversion rate (86%), from a 10% formic acid fed at the flow rate of 5 mL/min. High reaction temperature improved the conversion of formic acid feed at little expense of H 2 selectivity. The doping of Co in the Mo 2 C lattice improves the H 2 selectivity to 100% at 100–200 °C. A life time study showed the stability of this system by the remained high H 2 selectivity in formic acid decomposition. This work of using active carbon supported molybdenum carbides and high concentrated aqueous formic acid, opens up a new route for the portable H 2 generator using formic acid as a hydrogen storage material at no environmental risk.
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Mei Ma,Jia-qi Bai,Huangfei Liu,Ben Liu,Zhangkai Qian,Suiqin Li,Jingshuai Chen,Mengdie Cai,Song Sun
The preparation of methyl-substituted amines by direct N-methylation of amines with CO2/H2 is an important reaction for CO2 utilization and organic synthesis. However, the design and construction of effective and stable non-noble-metal catalysts for this reaction remain challenging. Here, a cheap non-noble-Cu-based catalyst was prepared and applied in the direct N-methylation reaction of N-methylaniline with CO2 and H2. 5%Cu-ZnO(3.75%)/TiO2 showed 98.8% yield with an initial TOF of 7.7 h–1 after 24 h under 453 K, 1.5 MPa CO2, and 4.5 MPa H2, which was superior to 5%Cu/TiO2, 5%Cu/ZnO, and reported Cu-based catalysts. Furthermore, 5%Cu-ZnO(3.75%)/TiO2 can be reused at least four times and applied to the direct N-methylation of various amines with excellent selectivity. The various characterizations and experimental results showed that Cu0 was the active site, and 5%Cu-ZnO(3.75%)/TiO2 exhibited the largest surface Cu0 amount, thereby contributing to superior catalytic performance. The reaction mechanism of the direct N-methylation reaction of N-methylaniline with CO2 and H2 was proposed based on spectroscopic studies, kinetic studies, and control experiments. The reaction proceeded with the HCHO and N-methylformanilide intermediates, and the formation of HCHO from H2 and CO2 was the rate-determining step.
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Xiying Jia,Yi Wei,Renhao Si,Cheng Wang,Pengzi Guo,Jianbing Ji
The Ni was dissolved as metal fog for homogeneous catalytic pyrolysis cellulose to produce H 2 -rich syngas in the molten carbonates. The Ni atoms firstly contact with CO 3 2− to form NiCO 3 in molten carbonate, then quickly decomposes into nickel oxide . The undissolved Ni atoms agglomerate with nickel oxide and remained nickel carbonate to synthesize metal cluster. The XRD and ex-situ Raman spectroscopy indicate that the oxidation state of the catalyst is between 0 (Ni sample) and +2 (NiO sample), meanwhile the TEM proposed that smaller particle size (50 nm) and higher dispersion of catalyst compared with raw Ni powder. Ni metal fog formed are expected to maximizing the production of H 2 -rich syngas by catalyzing cleavage of C–C and C–H bonds, which further contributes to tar cracking and water-gas shift reaction. The molten carbonate together with Ni metal fog pyrolysis cellulose achieved the maximum hydrogen yield of 289.16 ml/g-cellulose at 575 °C. A recycling study indicated that the hydrogen generated after five recycling cycles of the system was still maintained 289.05 ml/g-cellulose.
✓ 已验证
产品关联
DOI
高影响因子
Green Energy & Environment
·
2024
·
IF 10.7
Yi-lei Li,Xu-jia Liu,Yun-biao Wang,Ying Liu,Rui-hong Liu,Hui-ying Mu,Ying-juan Hao,Xiao-jing Wang,Fa-tang Li
Adjusting the interfacial transport efficiency of photogenerated electrons and the free energy of hydrogen adsorption through interface engineering is an effective means of improving the photocatalytic activity of semiconductor photocatalysts. Herein, hollow ZnS/NiS nanocages with ohmic contacts containing Zn vacancy (V Zn -ZnS/NiS) are synthesized using ZIF-8 as templates. An internal electric field is constructed by Fermi level flattening to form ohmic contacts, which increase donor density and accelerate electron transport at the V Zn- ZnS/NiS interface. The experimental and DFT results show that the tight interface and V Zn can rearrange electrons, resulting in a higher charge density at the interface, and optimizing the Gibbs free energy of hydrogen adsorption. The optimal hydrogen production activity of V Zn -ZnS/NiS is 10,636 μmol h −1 g −1 , which is 31.9 times that of V Zn -ZnS. This study provides an idea for constructing sulfide heterojunctions with ohmic contacts and defects to achieve efficient photocatalytic hydrogen production.
✓ 已验证
产品关联
DOI
高影响因子
MATERIALS SCIENCE IN SEMICONDUCTOR PROCESSING
·
2024
·
IF 4.2
Min Yuan,Ke Huang,Dongqing Dai,Hongfei Yin,Wei Zhao,Yixin Jiang,Yahui Feng
The integration of heterogeneous photocatalysts has emerged as a promising approach to boost the effectiveness of photocatalytic reactions for hydrogen evolution. In this study, we explore the synergistic effects of Ti 3+ -TiO 2 /P-doped g-C 3 N 4 heterojunctions on the enhancement of visible light-induced hydrogen generation efficiency. The photocatalytic hydrogen evolution performance of the as-prepared TPCN100 (280.38 μmol g −1 h −1 ) surpasses that of pristine P-doped g-C 3 N 4 (34.89 μmol g −1 h −1 ) and Ti 3+ -TiO 2 (39.71 μmol g −1 h −1 ) by factors of 8.0 and 7.1 respectively. Through a comprehensive investigation of the structural, electronic, and photocatalytic properties, the underlying mechanisms accountable for the observed enhancement in efficiency within the heterojunction system were elucidated. Based on the in-situ X-ray photoelectron spectrometer (XPS) examination, measurement of band edge, and electron paramagnetic resonance (EPR) analysis, the S-scheme photocatalytic mechanism was proposed. The integration of Ti 3+ -TiO 2 and P-doped g-C 3 N 4 offers new insights into the design of advanced photocatalytic materials for sustainable energy applications.
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2012
·
IF 5.625
Ting Bao,Zhongkui Zhao,Yitao Dai,Xiaoli Lin,Ronghua Jin,Guiru Wang,Turghun Muhammad
CO preferential oxidation (PROX) reactions were performed over the supported Co 3 O 4 -CeO 2 catalysts on modified activated carbon (AC) for eliminating the trace CO from H 2 -rich gases. The effects of support modification by H 2 O 2 oxidation treatment , catalyst calcination temperature, Ce/Co atomic ratio ( n Ce/Co ), Co 3 O 4 -CeO 2 loading and reaction parameters on catalytic properties of the Co 3 O 4 -CeO 2 /AC catalysts were investigated. Various characterization techniques like scanning electron microscopy (SEM), X-ray diffraction (XRD) and H 2 temperature-programmed reduction (H 2 -TPR) were employed to reveal the relationship between catalysts nature and catalytic performance. Results illustrate that the supported Co 3 O 4 -CeO 2 catalyst on modified AC exhibits excellent catalytic properties, which highly depends on dispersity and reducibility of Co 3 O 4 affected by the time of support treatment ( t p ), calcination temperature, n Ce/Co and loading. The supported 35 wt% Co 3 O 4 -CeO 2 catalyst (1:8 of n Ce/Co ) on the modified AC with H 2 O 2 oxidation treatment for 6 h demonstrates the best catalytic properties and the almost complete CO transformation takes place in a wide temperature range of 125–190 °C. Moreover, it is also found that the developed catalyst exhibits an outstanding catalytic stability, and 100% CO conversion can be maintained as the time on stream evolutes up to 1800 min even in the presence of CO 2 and H 2 O in the feed. The optimized Co 3 O 4 -CeO 2 /AC may be a robust and promising catalyst for eliminating trace CO from H 2 -rich gases.
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）