FUEL
·
2012
·
IF 3.248
Tao He,Yuxin Wang,Pengjie Miao,Jianqing Li,Jinhu Wu,Yunming Fang
Deep hydrogenation of aromatics is an important reaction in modern oil refinery. The key of an aromatic hydrogenation unit is high active, sulfur resistant hydrogenation catalyst. In this paper, the catalytic performance of a newly developed hydrogenation catalyst, platinum supported on mesoporous ZSM-5 (Pt/MZ-5), was tested in naphthalene (model compound of light cycle oil) hydrogenation. Pt/ZSM-5 and Pt/Alumina were used as reference. In some experiments, dibenzothiophene (DBT) was added to test the sulfur tolerance of catalysts. In the absence of DBT, Pt/MZ-5 and Pt/Alumina showed much higher hydrogenation activities and decalin selectivity than Pt/ZSM-5. The selectivity to decalin exceeds 97% over Pt/MZ-5 at temperature range between 523 and 573 K. Furthermore, Pt/MZ-5 shows better sulfur resistance than that of Pt/Alumina. In the presence of 3000 ppm dibenzothiophene, the selectivity of decalin over Pt/MZ-5 was only slightly dropped to 89.4% at 573 K, which is much higher than that of Pt/Al 2 O 3 (51.4%). The excellent catalytic performance and sulfur tolerance of Pt/MZ-5 were attributed to the combination of high acidity and mesoporous structure in MZ-5.
研究领域:
催化化学
·
石油炼制工程
✓ 已验证
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2024
·
IF 8.1
Shun Wang,Wen Jiang,Yifeng Zheng,Guoping Xiao
Surface and interface engineering as an efficient and controllable strategy in designing electrode structure has been widely investigated for achieving high catalyst activity and durability of robust electrodes in solid oxide cells (SOCs). The constructed heterojunction structures favor expedited charge transfer and promote the catalytic reaction. Anti-coking La 0.75 Sr 0.25 Cr 0.5 Mn 0.5 O 3-δ (LSCM)-based fuel electrodes are considered as promising candidates for alternative Ni-based cermet electrodes in solid oxide electrolysis cell (SOEC), however, they suffer from insufficient electrocatalytic activity for CO 2 electrolysis. Herein, Mn-containing Pr 0.6 Sr 0.4 FeO 3-δ (Pr 0.6 Sr 0.4 Fe 0.8 Mn 0.2 O 3-δ , PSFM) nanoparticles with excellent catalyst activity are synthesized and epitaxially grown on the surface of LSCM via infiltration technique. The spontaneous connected interface can provide direct tunnel for oxygen ion and electron transport along the (110) plane of LSCM. Meanwhile, this interface promotes an increase in oxygen vacancies and enhances both surface oxygen exchange and bulk oxygen diffusion capacities. These improvements are advantageous for CO 2 adsorption and carbonate dissociation at three phase boundaries (TPBs), leading to a significant enhancement in the kinetics of CO 2 reduction reaction. The electrolyte-supported single with PSFM/La 0.75 Sr 0.25 Cr 0.5 Mn 0.5 O 3-δ -Gd 0.1 Ce 0.9 O 2-δ (LSCM-GDC) fuel electrode exhibits an impressive current density of 1.09 A cm −2 at the applied voltage of 1.5 V and 800 °C, which increases by approximately 336 % than that of LSCM-GDC. In addition, the atomic arrangement enables in-situ formation of PSFM by trapping of surface Sr/Mn atoms on the LSCM surface, avoiding Sr segregation and enhancing the resistance to sulfur poisoning. This study demonstrates a strategy for achieving the enhanced CO 2 electrolysis performance and sulfur tolerance by engineering highly active interface.
研究领域:
材料科学
·
能源化学
·
催化反应
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Jiabin Ji,Congyun Zhang,Xianfeng Yang,Fanxin Kong,Chuanqiang Wu,Huimei Duan,Dongjiang Yang
Improving the sulfur-resistance of low-temperature methane combustion catalysts is great important for industrial applications. Electronic engineering of catalyst active sites is effective in tuning the catalytic performance. Herein, IrPt 0.5 /TiO 2 catalysts with electron-rich Ir structures modulated by Pt exhibit excellent low temperature sulfur-resistance towards methane combustion. The integrated characterization coupled with density functional theory calculations reveal that the strong electronic interaction between Ir and Pt induces the formation of electron-rich Ir structures. The electron-rich Ir structures with more defective oxygen vacancy and better redox ability greatly boost the adsorption and activation of O 2 while suppress SO 2 adsorption on the catalyst surface, leading to excellent sulfur tolerance towards methane combustion. This work highlights a practical electronic engineering strategy to tune the electron structure of Ir active sites for the development of practical methane oxidation catalysts.
研究领域:
催化化学
·
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2015
·
IF 7.435
Dongting Yue,Taiyang Zhang,Miao Kan,Xufang Qian,Yixin Zhao
The sulfur tolerant Mo 3 S 13 2− /BiOBr nanocomposite photocatalysts were facilely fabricated by a hydrothermal method. The characterizations including X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), energy dispersive X-ray spectrometry (EDS), UV–vis diffuse reflection spectroscopy (DRS) and photoluminescence (PL) investigate the structures, elemental composition, morphologies and photocatalytic activities of Mo 3 S 13 2− /BiOBr nanocomposite. The 5.0 wt% Mo 3 S 13 2− /BiOBr composite sample showed highest visible-light-driven photocatalytic activity for decolorization of organic dyes including Rhodamine B (RhB) and sulfure containing methylene blue (MB). The decolorization of RhB was dominated by the direct hole and the generated O 2 − radicals oxidation process . Our 5.0 wt% Mo 3 S 13 2− /BiOBr nanocomposite exhibited comparable photocatalytic activity as the state of art 1 wt% BiOBr/Pt composite for photocatalytic decolorization of RhB. The 5.0 wt% Mo 3 S 13 2− /BiOBr composite possessed better sulfur resistance than 1.0 wt% Pt/BiOBr composite.
研究领域:
材料科学
·
环境科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
AICHE JOURNAL
·
2024
·
IF 3.5
Zhongzhe Wei,Guanglu Dong,Long Zhao,Songtao Huang,Molin Xia,Wei Huang,Ming Jiang,Zhixiang Yang,Zihao Yao,Jianfeng Li,Jianguo Wang
Given that the retention of nitrogen readily renders active site poisoning, designing versatile catalysts characterized by notable selectivity and even resistance to poisoning for alkyne semi-hydrogenation under nitrogen-containing conditions is considerably challenging. In this article, oxanilide-decorated Pd/C (Pd/C-oxa) catalyst is facilely synthesized by leveraging impregnation-coordination, which exhibit remarkable performance in the semi-hydrogenation of nitrogen-containing alkynes, with ultrahigh turnover frequency (TOF) of 15,831 h −1 and selectivity of 97.2%. Strikingly, it still sustains TOF of 12,137 h −1 in a sulfur-containing system, demonstrating distinguished tolerance to sulfur. Comprehensive studies corroborate that oxanilide tunes the electron density of Pd by constructing metal–ligand electronic interactions, facilitating hydrogen activation. Simultaneously, the reaction microenvironment is optimized, which effectively promotes the desorption of nitrogen-containing olefins and attenuates the aggregation of nitrogen on the Pd surface. This strategy is universal and holds promising industrial applications, making it appropriate for use in commercial Pd/C catalysts as well.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Xiaoqiang Wang,Yue Liu,Zhongbiao Wu
In this paper, the Cu-Ce based catalyst using NbOPO 4 (Nb-P) as support was firstly employed for selective catalytic reduction (SCR) of NO by NH 3 . The experimental results had illustrated that such catalyst exhibited well SCR activity and N 2 selectivity within a wide temperature range of 200–450 °C. These superior performances could be mainly attributed to its improved textural properties and strong acidity derived from NbOPO 4 support. More importantly, the sulfur tolerance of the NbOPO 4 supported Cu-Ce sample was found greatly improved compared to TiO 2 and Ti-Nb supported samples, where above 80% SCR activity of Cu-Ce/Nb-P sample was obtained at 250 °C after 10 h reaction running in the presence of 100 ppm SO 2 . This fact was the result of the enhanced acidity and the strong interactions between Cu-Ce oxides and NbOPO 4 support, which could prevent the surface oxygen species from sulfation by SO 2 . As such, these oxygen species strongly associated with NbOPO 4 support still could activate adsorbed NH 3 to fulfill the SCR reaction cycle, leading to its better sulfur resistance. The work would provide some enlightenments to the development of NH 3 -SCR catalysts with high sulfur resistance at medium-high temperature.
研究领域:
催化化学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2019
·
IF 4.63
Zhiwei Wang,Sha Li,Shaohua Xie,Yuxi Liu,Hongxing Dai,Guangsheng Guo,Jiguang Deng
Volatile organic compounds (VOCs) cause damage to atmospheric environment and human health. Supported noble metal catalysts are widely used to control VOCs emissions. The high cost, and low H 2 O-, CO 2 -, and SO 2 -resistance of such catalysts are worthy to be improved. Herein we fabricated Ce-, V-, or W-doped TiO 2 supported ultralow loading Pt catalysts via the in-situ molten salt method, and evaluated their catalytic performance for acetone (major pollutants in pharmaceutical industry) removal. Under the present reaction conditions, all the catalysts exhibited high catalytic activity and stability for acetone oxidation , with the temperature required 90% acetone conversion being of 245 °C over 0.57 wt% CeO 2 -0.05 wt% Pt/TiO 2 . The doping of Ce, V, or W enhanced the H 2 O-, CO 2 -, and SO 2 -tolerance ability of 0.05 wt% Pt/TiO 2 . More than 85 %85%, 70%, or 60% of acetone could be removed even in the presence of 20 vol% water vapor, 10 vol% CO 2 , or 100 ppm SO 2 , respectively. The improvement in SO 2 -tolerance ability was due to the inhibition of SO 2 adsorption and oxidation activity as well as Ti(SO 4 ) 2 or TiOSO 4 formation. Acetone complete oxidation over 0.57 wt% CeO 2 -0.05 wt% Pt/TiO 2 would follow the pathway: adsorbed acetone molecules → acetic acid and formic acid → carbonate species → CO 2 and H 2 O. The present supported Pt catalysts might be suitable for oxygenated VOCs removal.
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 COLLOID AND INTERFACE SCIENCE
·
2019
·
IF 6.361
Xiaoqiang Wang,Yue Liu,Weiyuan Yao,Zhongbiao Wu
In this paper, a series of Sb modified CeZr 2 O x mixed oxides (Sb y CZ) were synthesized by citrate method for the selective catalytic reduction of NO with ammonia (NH 3 -SCR). Experimental results exhibited that the Sb addition could bring a great improvement of SCR activity at 200–360 °C owing to the enhancement in surface area , redox ability and surface acidity . More importantly, the sulfur tolerance of the catalyst with proper Sb loading contents was dramatically improved. For instance, above 85% deNO x efficiency was retained over Sb 0.5 CZ catalyst after 24 h reaction in the presence of 100 ppm SO 2 and 5 vol.% H 2 O. As for pure CeZr 2 O x and the catalysts with low Sb loading contents, the serious accumulation of ammonium sulfates resulted in the deactivation after SO 2 exposure. However, with excessive Sb addition, more labile oxygen readily reacted with SO 2 and the redox cycle was then disrupted, leading to the decrease of SCR activity. With an appropriate Sb loading contents, the sulfate species preferentially formed around Sb cations could restrain the further consumption of oxygen species in Ce-O-Ce or Ce-O-Zr mode by SO 2 via a space confinement effect. Thus, a certain amount of labile oxygen was preserved to drive the SCR reaction, thereby enhancing the sulfur tolerance of the catalyst.
研究领域:
催化
·
环境化学
·
材料科学
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
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.
研究领域:
催化化学
·
环境科学
✓ 已验证
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Manli Wang,Longsheng Cao,Zhicheng Liu,Wenbing Yang,Shucheng Sun,Ming Hou,Zhigang Shao
SO 2 , one of the considerable air pollutants, exhibits a stronger binding affinity with Pt when compared to O 2 , thereby inducing irreversible degradation of the Oxygen Reduction Reaction (ORR) catalyzed by Pt-based catalysts. Despite this detrimental phenomenon, scarce investigations have delved into the realm of contaminant-tolerant catalysts, and so far, no effective SO 2 -tolerant catalysts have been proposed. To meet this challenge, we designed and synthesized a core–shell structure catalyst equipped with a dual protection mechanism. This was achieved through the in-situ polymerization of aniline monomers, concomitantly reducing Pt 2+ . The resulting shell effectively hinders the transmission of SO 2 to the active sites of Pt, while permitting the unimpeded transmission of O 2 . Simultaneously, the intermetallic core inhibits the adsorption of SO 2 . Therefore, this catalyst exhibits exemplary ORR activity coupled with exceptional resistance to SO 2 resistance. In particular, the PtFe@FeNC/C-10 catalyst, optimized in terms of the quantity of added aniline, demonstrates a mass activity 1.84 times greater and a specific activity 4.03 times higher than that of commercial Pt/C catalysts. Following exposure to SO 2 -induced poisoning, the E 1/2 value of the PtFe@FeNC/C-10 catalyst undergoes a decrease of only 51.7 mV, lower than that observed for the commercial Pt/C catalyst (92.0 mV). Moreover, the results of an accelerated durability test affirm the superior stability of PtFe@FeNC/C-10 in comparison to commercial Pt/C. This stability advantage is attributed to the protective carbon shell, which effectively prevents the detachment and agglomeration of Pt nanoparticles .
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2020
·
IF 16.683
Zhiquan Hou,Lingyun Dai,Yuxi Liu,Jiguang Deng,Lin Jing,Wenbo Pei,Ruyi Gao,Yuan Feng,Hongxing Dai
Catalytic oxidation is one of the effective pathways for completely eliminating volatile organic compounds (VOCs) emitted from industrial and transportation activities. Meanwhile, single-atom catalysts have excellent application prospects in numerous reactions due to their high metal atomic utilization efficiency. In this work, we adopted a novel strategy to prepare an active Pd/Co single-atom catalyst (i.e., Pd 1 Co 1 /Al 2 O 3 ) for benzene oxidation. The successful formation of the atomically dispersed palladium and cobalt species on Al 2 O 3 was verified by the aberration-corrected high-angle annular dark-field scanning transmission electron microscopy and X-ray absorption fine structure. By the in situ temperature-programmed techniques and in situ diffuse reflectance Fourier transform infrared spectroscopy, we observed a double effect of the palladium and cobalt oxide active sites, resulting in an enhanced performance for benzene oxidation. A benzene conversion of 90 % was achieved over the Pd 1 Co 1 /Al 2 O 3 catalyst at 250 °C and a space velocity of 40,000 mL/(g h). Interestingly, the catalyst also possessed enhanced sulfur resistance performance. The good regeneration ability of the active sites in the catalyst was due to the single-atom dispersion of Pd and Co. In addition, we deduce that benzene oxidation might occur over Pd 1 Co 1 /Al 2 O 3 via a pathway of benzene → cyclohexadiene → phenol → quinone → maleate → acetate → CO 2 and H 2 O. We believe that the obtained results can provide a useful idea for rationally designing the double active site single-atom catalysts and understanding the mechanism of VOCs oxidation.
研究领域:
催化化学
·
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2023
·
IF 7.4
Yuxin Sun,Yunshuo Wu,Yarong Bai,Xuanhao Wu,Haiqiang Wang,Zhongbiao Wu
Iridium nanocatalysts are ideal candidates for the selective catalytic reduction of NO x by CO (CO-SCR) in excess oxygen. Here, a high-performance Ir nanocatalyst supported on natural halloysite nanotubes (HNTs) was applied for the CO-SCR. The HNTs loaded with only 0.5 wt% Ir achieved 78 % NO x conversion at 250 °C in the presence of 5 % O 2 , which was the highest among catalysts with varied Ir loadings or reduction temperatures. It also possessed an excellent SO 2 and H 2 O tolerance during longevity tests. An interesting SO 2 -enhanced CO-SCR long-term stability was observed, which was ascribed to the inhibitory effects of SO 2 on the side reaction between CO and O 2 . The loading amount and the reduction temperature could modulate the size of Ir nanoparticles and the percent of Ir 0 , which were two key factors determining the CO-SCR activity. DRIFTS characterizations and DFT calculations coherently revealed the favorable adsorption sites of CO (top) and NO (hcp) on Ir nanoparticles. The Ir atoms served as a charge transfer bridge from the C atom of CO to the N atom of NO, leading to the enhanced breakage of N-O bonds. This work provides Ir/HNT as a promising CO-SCR material with high performance and robustness to tackle NO x pollution.
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
危险品化学品经营许可证（带存储）