JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Jianwen Lai,Hongbo Qi,Yunfeng Ma,Xiaoqing Lin,Xiaoying Wang,Zhongkang Han,Heidelore Fiedler,Xiaodong Li
Cerium is widely used as a modifier to enhance the catalytic performance of the selective catalytic reduction (SCR) catalysts due to its exceptional low-temperature properties. However, the effects of different cerium precursors on catalytic performance remains unclear. In this study, VO x -WO x /TiO 2 catalysts are modified using Ce(NO 3 ) 3 ·6H 2 O (cata-N), CeO 2 (cata-O), and Ce(OH) 4 (cata-OH), and their synergistic removal of NO x and chlorobenzene (CB), as well as their resistance to water and sulfur poisoning, were systematically investigated. Among the tested catalysts, cata-N demonstrated superior CB (45.0–93.3 %) and NO x (31.9–90.37 %) removal efficiencies under synergistic conditions, along with excellent water resistance (T 90 = 193 °C with 5 % H 2 O). In contrast, cata-OH exhibited the highest sulfur resistance, maintaining a denitrification efficiency of 20 % after 10 h of sulfur exposure, compared to 9 % for cata-N and 8 % for cata-O. Characterization revealed that Ce(NO 3 ) 3 ·6H 2 O improved cerium dispersion, leading to enhanced the redox properties and acidity (especially Brønsted acid sites (BAS)) in cata-N. Density functional theory (DFT) calculations and In-situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy ( In-situ DRIFTS) results revealed that the well-dispersed cerium atoms contributed additional BAS in the form of Ce–OH, while also forming Ti–O–Ce bonds. These Ti–O–Ce bonds facilitated the formation of Ti–OH on the TiO 2 surface. Ti–OH significantly enhanced the adsorption of NH 3 and CB, thereby promoting both the NH 3 -SCR and CB oxidation processes. This study offers new insights into the role of cerium precursors and provides a practical strategy for tuning BAS of catalysts in multiple pollutants removal.
研究领域:
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
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
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化学工程
·
表面科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Mingqiang Chen,Zhiwei Yang,Haosheng Xin,Yishuang Wang,Defang Liang,Chang Li
As a major constituent of renewable biomass, conversion of cellulose to high-value chemicals presents a promising strategy. Herein, we designed a multifunctional Ni@C/WOx catalyst for direct cellulose conversion to ethylene glycol. This catalyst exhibited excellent stability while achieving a high ethylene glycol yield (69.4%). Graphene-encapsulated metal Ni stabilized hydrogenation activity and minimized metal leaching. The interaction between Ni@C and WOx facilitated the reduction of WOx and increased the formation of W5+ species. Characterization by electron paramagnetic resonance (EPR), X-ray photoelectron spectroscopy (XPS), NH3-TPD, and Py-IR confirmed that W5+ formation induces oxygen vacancies and acid sites on the catalyst support surface. At 30% Ni loading, strong metal–support interactions maximized the W5+ concentration and oxygen vacancy, enhancing the C–C bond cleavage efficiency. Consequently, the synergistic effect between Ni@C and WOx effectively facilitates key steps in cellulose conversion to ethylene glycol: cellulose hydrolysis, glucose retro-aldol condensation, and glycolaldehyde hydrogenation. The understanding of these structure–performance relationships has provided new ideas for the green and sustainable production of high-value-added chemicals from cellulose.
研究领域:
催化
·
绿色化学
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生物质转化
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材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2024
·
IF 6.5
Jingyuan Shang,Yan Li,Yiwen Hu,Tong Zhang,Ting Wang,Jinqing Zhang,Hao Yan,Yibin Liu,Xiaobo Chen,Xiang Feng,Xingong Zhang,Chaohe Yang,De Chen
Chemical upcycling through catalytic hydrocracking to fuels has potential to mitigate the serious environmental issues caused by plastic waste. Herein, non-noble tungstate-zirconia supported nickel catalyst (Ni/WO x -ZrO 2 ) with tunable Brønsted/Lewis (B/L) ratio was firstly proposed for the hydrocracking of low-density polyethylene (LDPE), which achieves hydrogenation/dehydrogenation on Ni sites and cracking/isomerization on WO x -ZrO 2 , respectively. Excellent 100 % LDPE conversion with 76.9 % liquid yield was achieved, which is comparable to noble Ru-based and Pt-based catalysts. Quantitative linear relationship between B/L ratio and hydrocracking performance was established, and the key to boost performance was keenly controlling the volcanic-shape relationship between surface WO x density and B/L ratio of catalyst. Moderate WO x surface density with higher B/L ratio enhances LDPE hydrocracking, and inhibits the hydrogenation of the primary products. However, excessive WO x polymerized and formed WO 3 crystals, compensating acid sites and inhibiting LDPE hydrocracking. This work is of prime scientific and industrial significance to the rational design of catalysts for industrial plastic hydrocracking.
研究领域:
催化
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环境科学
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材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2024
·
IF 4.1
Wenjin Li,Wanting Zhao,Qizhen Luo,Wenzhe Xiao,Xiaoning Wang,Yuting Shi,Jian Sun
High photogenerated carrier recombination inhibits the widespread application of graphite-phase carbon nitride (g-C 3 N 4 ). Construction of junctions is an effective strategy but still under challenges, such as tedious procedure and limited efficiency. Herein, WO x /1D g-C 3 N 4 /2D g-C 3 N 4 multi-junction with enhanced separation of photogenerated carriers was one-pot integrated through in-situ “PTA-Mel” ionic microenvironment by mixing phosphotungstic acid (PTA) and melamine (Mel). Protonated Mel by PTA contributed to the formation of 1D g-C 3 N 4 and the decomposition of [P(W 3 O 40 ) 4 ] 3- produced WO x . 1D g-C 3 N 4 and WO x with oxygen-vacancy deficient provided channels and caves for photoelectrons transfer, respectively. Compared with pure g-C 3 N 4 , the degradation rate constants of Rh B and tetracycline hydrochloride (TC) by WO x /1D g-C 3 N 4 /2D g-C 3 N 4 are 2.34 and 1.45 times high respectively due to the excellent visible light absorption and improved photogenerated carrier separation. This method could be extended to the design of multiple heterojunctions in one photocatalyst through a facile process.
研究领域:
材料科学
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环境科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
·
2020
·
IF 12.35
Haiyong Wang,Haosheng Xin,Chiliu Cai,Changhui Zhu,Zhongxun Xiu,Qiying Liu,Yujing Weng,Chenguang Wang,Xinghua Zhang,Shijun Liu,Zifang Peng,Longlong Ma
Keto-alcohols, which are traditionally produced from fossil resources with multisteps, are considered as important intermediates for diversified high-value-added fine chemical synthesis due to their involved carbonyl and hydroxyl groups. Herein, direct cellulose hydrogenolysis to C3-C4 keto-alcohol products (hydroxyacetone and 1(3)-hydroxy-2-butanone) was achieved over Ni-WOx/C catalysts with an W/Ni atom ratio of 1.0–5.0. The keto-alcohol yield was proposed to strongly depend on the W/Ni ratio and the catalyst annealing temperature. The highest keto-alcohol yield of 63% was obtained at the optimal balance of basic/acidic WOx species and metallic Ni. The introduction of Ni facilitated the formation of the basic W5+ sites, which enhanced the formation of basic sites at the Ni-WOx interface. The synergistic effect between the basic W5+ and acidic oxygen vacancy (Vö) could activate the target C–O/C═O bonds, promoting the isomerization of glucose and C3-C4 aldehyde intermediates with the assistance of the interfacial Ni. The cooperative adsorption of the −OH and −C═O groups at the Ni-O-W-Vö interface stabilized the adjacent ketone and hydroxyl groups and kept the other hydroxyl groups for hydrogenolysis, obtaining the final C3-C4 keto-alcohols. This work expanded the application of cellulosic biomass, enabling the green and sustainable synthesis of the high-value C3-C4 keto-alcohol products using lignocellulosic biomass as a raw material.
研究领域:
化学工程
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催化
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绿色化学
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可再生能源
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Ying Xu,Genkuo Nie,Xiao Jiang,Hongyu Wang,Guihua Yang,Ziyi Yan,Ji-Jun Zou,Hailong Yu,Shitao Yu,Yu Liu
Metal-metal oxide catalysts are robust in selective hydrodeoxygenation of biomass derives. Herein, 1-hexanol in total yield about 76 % is firstly achieved by high selective hydrodeoxygenation of 5-hydroxymethylfurfural over Ni/MCM-41 and Pt-WO X /t-ZrO 2 . By controlling the amount ratio of Ni/Ni 2+ to 0.46, a 99.9 % yield of 2,5-tetrahydrofurandimethanol was achieved from 5-hydroxymethylfurfural by Ni/MCM-41. Subsequently high yield of 76 % of 1-hexanol was obtained by competing pathways of tandem reactions beginning at SN2 reaction at the epoxy atom of 2,5-tetrahydrofurandimethanol to enol/tautomer intermediates and ending with controllable selective hydrogenation. The reaction mechanism is explored and the reaction-oriented regulation is realized by the additional strong BrÖnsted acid sites generated by electron transfer from W to Pt and the appropriate amount of Pt 0 sites of Pt-WO X /t-ZrO 2 , where the ratios of W 5+ /W 6+ and Pt 0 /Pt 2+ are 0.31 and 4.58 respectively. This work provides a new and green method for the synthesis of 1-hexanol and expands the utilization of metal–metal oxide in making value-added products using sustainable feedstocks.
研究领域:
催化
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化学工程
·
绿色化学
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生物质转化
✓ 已验证
产品关联
DOI
高影响因子
ACS Omega
·
2021
·
IF 3.512
Yixuan Huang,Guangcai Zhang,Qinhui Zhang
In the present work, an efficient and stable WOX/MCM-41 solid acid catalyst was prepared by the wet impregnation method. The characterization of powder X-ray diffraction, transmission electron microscopy, ultraviolet–visible, H2 temperature-programmed reduction, X-ray photoelectron spectroscopy, NH3 temperature-programmed desorption, and N2 adsorption–desorption isotherms confirmed that the impregnation amount and calcination temperature of WOX speciation affected the dispersity and acidity of the resulting catalyst. This WOX/MCM-41 solid acid catalyst was subsequently applied in the ketalization reaction of glycerol and acetone to produce solketal. By catalyst screening and reaction condition optimization, WOX/MCM-41 obtained by impregnating 20 wt % and calcining at 350 °C exhibited the highest solketal yield and catalytic stability.
研究领域:
催化
·
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Sustainable Chemistry & Engineering
·
2023
·
IF 8.4
Man Yang,Yuxiang Jiao,Jianglin Duan,Keying Wu,Hailiang Song,Shaodong Sun,Yujing Ren
Taking the background of the ambiguous role of oxophilic metal oxide in metal-acid bifunctional catalysts for the important field of tetrahydrofurfuryl alcohol (THFA) hydrogenolysis, a linear relationship between the W═O/W–OH content in sub-nano-Rh-supported WOx and 1,5-pentanediol (1,5-PeD) yields from THFA hydrogenolysis has been established. It reveals that the higher reduction temperature promotes the surface Rh/W ratio. Thus, hydrogen spillover is facilitated, leading to more surface W═O structures and thereby more in-situ-reduced W–OH generation. W–OH structures work as the active sites to provide in situ Brønsted acid, resulting in enhanced selective activation for secondary C–O bonds of THFA. This discovery reveals the unique role of the surface structure on oxophilic metal oxide in chemoselective hydrogenolysis of the secondary C–O bond in polyols.
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
高影响因子
FUEL
·
2021
·
IF 6.609
Antony Rajendran,Hong-Xia Fan,Tian-You Cui,Jie Feng,Wen-Ying Li
Designing an efficient and selective catalyst for the ultra-deep sulfur removal from liquid fuels under mild conditions is vibrant in environmental catalysis. This work reports the preparation of catalysts, i.e., WO x -based active sites generated on SnO 2 , for the sulfur removal from model diesel via biphasic oxidative desulfurization (ODS). The different active species generated on SnO 2 such as monomeric and polymeric WO x species, and crystalline WO 3 are characterized. Besides being the support, SnO 2 adsorbs the sulfur compounds from the oil phase and boosts the ODS performance. No significant change in the ODS activity of WO x @SnO 2 is observed in the presence of intrusive nitrogen and aromatic compounds. The order of ODS activity towards different sulfur compounds is dibenzothiophene (DBT) > 4,6-dimethyl DBT > benzothiophene. While using SnO 2 with a higher surface area (96.5 m 2 /g) instead of that with a lower surface area (19.2 m 2 /g), the formation of highly efficient polymeric WO x species is enhanced. Consequently, the turn over frequency is augmented from 10.99 to 43.23 h −1 , which is closely a 4-fold increase. The polymeric WO x species produced on SnO 2 having the higher surface area are visualized by HAADF-STEM analysis. Scalable preparation and the higher turnover frequency of the present catalyst can develop a promising catalytic system for the ODS.
研究领域:
环境催化
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
·
2026
·
IF 13.6
Xiaoru Wang,Zhanwu Lei,Jicong Yan,Penglong Wang,Ruifeng Chong,Fuping Tian,Tao Hu,Ruiguo Cao,Xiang Wang
Developing non-noble metal catalysts for hydrocracking polyolefins is a promising yet formidable challenge for upcycling waste plastics in practice. Herein, we report a NiW/WOx (2 < x < 3) catalyst, which accomplishes polyolefin hydrocracking at 250 °C, yielding a liquid product of about 73 wt % and a gaseous product of about 22 wt %. The liquid fraction primarily consists of hydrocarbons in the C4–C25 range, with more than 77% falling within the jet-fuel-range components (C8–C16). The gas product is dominated by branched C3–C6 hydrocarbons, characteristic of liquefied petroleum gas (LPG), with negligible carbon loss, such as methane and ethane.A sequence change from inactive to active, and back to inactive in polyolefin hydrocracking was found accompanying the reconstruction of the surface structure of the catalyst from Ni-doped WO3 to NiW alloy nanoparticles supported on WOx (NiW/WOx), and then to WO2-encapsulated NiW (NiW@WO2). The coexposure of NiW alloy nanoparticles and WOx is further demonstrated to be necessary for fulfilling the bifunctionality of the catalyst in hydrogen dissociation and C–C bond cleavage in polyolefin hydrocracking, and the absence of either will deactivate the catalyst.
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2015
·Vol. 5
·期 128
·106053-106060
·
IF 3.84
Jie Wang,Ting Qu,Minsi Liang,Zhenbo Zhao
In this work, we investigated the dehydration of fructose into 5-hydroxymethylfurfural using solid catalysts with microwave assistance in dimethyl sulfoxide. Five kinds of solid catalyst ZrO2, WOx/ZrO2, MoOx/ZrO2, SO42−/WOx–ZrO2 and SO42−/MoOx–ZrO2 were prepared and characterized by XRD, UV-DRS, FTIR, XPS, TEM, TPD, BET, and Raman and the surface acid amount was obtained by combining pyridine adsorption and UV spectrometry. The SO42−/WOx–ZrO2 catalyst was found be the most active catalyst, and a fructose conversion of 95.80% with 83.90% 5-HMF yield was obtained at 150 °C in a relatively short reaction time of 5 min. The value of the activation energy was comparable with previous values reported in the literature, implying that SO42−/WOx–ZrO2 was efficient for the dehydration of fructose to 5-HMF and that microwave radiation heating had a remarkable accelerating effect on the fructose conversion.
研究领域:
化学工程
·
催化科学
✓ 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）