CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Yanke Yu,Desheng Wei,Zhaojian Tong,Jinxiu Wang,Jinsheng Chen,Chi He
Ammonia (NH 3 ) is a critical component causing environmental problems like haze and water pollution. Selective catalytic oxidation of ammonia (NH 3 -SCO) to N 2 and H 2 O is a promising method to abate NH 3 emission. However, inferior SO 2 tolerance is still a tremendous challenge to be conquered for present NH 3 -SCO catalysts regarding practical applications. Application of materials which was difficult to be sulfated by SO 2 should be an effective way to solve this problem. Here, a ReO x -CuSO 4 /TiO 2 catalyst which coupled the advantages of ReO x (Rhenium oxides, supplying highly active adsorbed surface oxygen enhancing NH 3 -SCO reaction) and CuSO 4 (providing Brønsted acid sites inhibiting the formation of N 2 O) was rationally fabricated. Results indicated that ReO x -CuSO 4 /TiO 2 catalyst exhibited excellent catalytic performance in NH 3 -SCO with almost 100% of NH 3 oxidized at 300 °C (N 2 selectivity as high as 96%). Crucially, the composite catalyst exhibited incredible activity and stability under harsh reaction conditions toward SO 2 (600 ppm) and H 2 O (4.0 vol%) owing to the superior inhibition capability for SO 2 adsorption. In situ DRIFTS, in situ Raman and in situ XPS demonstrated that the NH 3 -SCO reaction over ReO x -CuSO 4 /TiO 2 catalyst mainly obeyed a N 2 H 4 reaction mechanism and oxidation–reduction circle between Re 7+ and Re 6+ played a vital role. Moreover, SO 2 would not affect this reaction mechanism on ReO x -CuSO 4 /TiO 2 catalyst. The knowledge and understanding reported could provide critical insights for the design and optimization of efficient materials for industrial NH 3 oxidative elimination.
研究领域:
催化化学
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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
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Cong Wu,Qinglong Liu,Yu Zhan,Wei Tan,Xiaoqian Wei,Qing Tong,Haiqin Wan,Lin Dong
Indoor volatile organic compounds (VOCs), represented by toluene, can pose a serious threat to human health. In this work, a series of Pd/TiO 2 catalysts with different surface structures ( i.e. , dispersion/valence of Pd species, surface Ti 3+ /oxygen defect concentration and Pd-TiO 2 interactions, etc. ) was constructed by various methods. It was found that the Pd/TiO 2 catalyst prepared by one-step reduction of NaBH 4 method (Pd/TiO 2 -N) with metallic Pd particles possessed more surface Ti 3+ /oxygen defects and stronger Pd-TiO 2 interaction than Pd/TiO 2 catalysts prepared by ethylene glycol reduction loading method (Pd/TiO 2 -E) and incipient wetness impregnation method (Pd/TiO 2 -I). Further photochemical characterizations and reaction mechanism study revealed that the relatively higher concentration of Pd 0 species on Pd particles, stronger Pd-TiO 2 interaction, and more surface Ti 3+ /oxygen defects on Pd/TiO 2 -N could facilitate the generation of more reactive oxygen species (ROS) under light irradiation. The partial oxidation of toluene to benzyl alcohol/benzaldehyde/benzoic acid and the subsequent ring-opening process were found to be highly determined by the valence states of Pd particles and the concentration of surface Ti 3+ /oxygen defects. This work provides instructive insights into the construction of highly efficient Pd/TiO 2 catalysts for the removal of indoor VOCs.
研究领域:
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
ENERGY & FUELS
·
2023
·
IF 5.3
Linghan Xia,Mengchen Wu,Yimeng Li,Hongyan Guo,Yonghong Cheng,Guodong Meng
As one of the most consensus goals around the world, reduction of carbon emissions has attracted huge attention from academic and industry communities for developing renewable energy sources and carbon capture techniques. Nonthermal equilibrium plasma catalysis has been proven to be a very promising way for CO2 conversion into high-value-added products; however, the synergistic catalytic mechanism between the plasma and various catalysts remains a challenge. In this work, we designed a reactor of atmospheric pressure glow discharge (APGD) plasma jet coupled with V2O5/TiO2 nanocomposite catalysts and studied the influence of V2O5 mass fraction, catalyst pretreatment, and reaction plasma parameters on the CO2 dissociation performance. Results showed that the designed reactor could introduce high-density plasma to the downstream area and maintain lower gas temperature, allowing the collaboration between APGD and the V2O5/TiO2 catalyst. The XRD analysis indicated that the solid solution phase TiVO4 could be formed in catalysts by V2O5 doping and reach a maximal content at a mass fraction of 30%, which determined the most excellent redox ability of the catalyst. The pretreatment of the as-prepared catalyst by Ar dielectric barrier discharge (DBD) plasma increased the oxygen vacancy density of the catalyst, thereby raising the conversion rate by 18.43%. Moreover, the transition regime between laminar and turbulent states was found to be the optimal configuration for CO2 dissociation. The reaction pathway was proposed for CO2 dissociation synergistically catalyzed by an APGD plasma jet and V2O5/TiO2. Ultimately, the maximum conversion of 14.88% and energy efficiency of 40.45% were simultaneously achieved, which were superior to the results of most atmospheric pressure plasmas. This work opens an avenue to develop plasma technology for sustainable CO2 utilization.
研究领域:
环境科学
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材料科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
MOLECULES
·
2023
·Vol. 28
·期 17
·6187
·
IF 4.6
Le Xu,Jiateng Chen,Pengcheng Zhao,Boxiong Shen,Zijian Zhou,Zhuozhi Wang
To promote the practical application of TiO2in photocatalytic toluene oxidation, the honeycomb aluminum plates were selected as the metal substrate for the loading of TiO2powder. Surface-etching treatment was performed and titanium tetrachloride was selected as the binder to strengthen the loading stability. The loading stability and photocatalytic activity of the monolithic catalyst were further investigated, and the optimal surface treatment scheme (acid etching with 15.0 wt.% HNO3solution for 15 min impregnation) was proposed. Therein, the optimal monolithic catalyst could achieve the loading efficiency of 42.4% and toluene degradation efficiencies of 76.2%. The mechanism for the stable loading of TiO2was revealed by experiment and DFT calculation. The high surface roughness of metal substrate and the strong chemisorption between TiO2and TiCl4accounted for the high loading efficiency and photocatalytic activity. This work provides the pioneering exploration for the practical application of TiO2catalysts loaded on the surface of metal substrate for VOCs removal, which is of significance for the large-scaled application of photocatalytic technology.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Catalysis
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2024
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IF 11.3
Hang Yu,Shanjun Mao,Bing Lu,Hao Wang,Xie Zhang,Menghui Qi,Ruiliang Gao,Yong Wang
Multicomponent reactions such as ammoxidation are highly desirable for chemical synthesis. The complicated reaction network and catalytic active sites involved, however, make it rather challenging for extensive structure–performance relationship investigations and subsequent rational design of an efficient catalyst. In this work, efficient VOx/TiO2 catalysts with concise components and exquisite structure design demonstrated 95% selectivity at 98% conversion under 2070 h–1 for 3-picoline ammoxidation. After clarifying that the oxidative dehydrogenation process is rate-limiting, we assumed that the abundance of reactive surface lattice oxygen at the interface of vanadium–titanium is the key to high productivity and suppression of oxidation side reactions since low reaction temperature is beneficial for enlarging the difference in rates of different energy barriers. In addition, rather than applying the traditional neutralization method with alkaline components, in situ formed V2O5 crystallite was subtly to cover the strong acid sites on VOx/TiO2 catalysts in that the strong adsorption of pyridine nitrogen in 3-cyanopyridine on strong acid sites can lead to severe hydrolysis side reactions.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2023
·
IF 8.4
Zhenlong Song,Yuzhen Hu,Song Li,Jianguo Liu,Xinghua Zhang,Longlong Ma,Lungang Chen,Qi Zhang
Valorizing lignin into valuable chemicals requires the selective breaking of a large number of C–O bonds found in the β–O–4 structure. In this study, we present a one-pot strategy that utilizes two NiO/TiO2 catalysts for the photocatalytic depolymerization of β–O–4 alcohols. The S-1.6%NiO/TiO2 catalyst is used for the dehydrogenation of β–O–4 alcohols at 450 nm. Then, the L-0.8%NiO/TiO2 catalyst is employed for the hydrogenolysis of β–O–4 ketones at 365 nm. Remarkably, the dehydrogenation–hydrogenolysis tandem reaction can be conducted in one pot, which affords high yields of ketones and phenols (up to 89%) from β–O–4 alcohols. Additionally, the L-0.8%NiO/TiO2 catalyst prepared in this article is the smallest NiO/TiO2 photocatalyst reported to date, and the size of NiO in the S-1.6%NiO/TiO2 catalyst is even small enough to enter the lattice of TiO2. We successfully regulated the reaction selectivity by controlling the loading method and the amount of NiO. Our work offers a promising solution for efficiently cleaving target bonds in lignin and provides insights into the design of efficient photocatalysts.
研究领域:
化学工程
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材料科学
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可再生资源转化
✓ 已验证
DOI
高影响因子
Energy Material Advances
·
2025
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IF 15.9
Xueke Wang,Yixuan Li,Jessica Nginyo,Daniela Iracelma Difuma Luis,Dong Cao,Zhiyong Deng,Weijie Cai
Reducing the greenhouse gas CO2 in the atmosphere and converting it into high-value-added syngas is regarded as a competitive strategy in line with green and sustainable development. Herein, a series of M/TiO2 (M = Cu, Co, Ni) catalysts were developed for photothermal CO2 reduction with bioethanol, and the synergistic mechanism between photocatalysis and thermocatalysis was deeply investigated. Systematic characteristics and photothermal ethanol dry reforming (EDR) testing results revealed the relevancy between catalytic behavior and microstructure properties of TiO2-supported catalysts. Notably, the Ni/TiO2 catalyst displayed superior catalytic behavior than Cu/TiO2 and Co/TiO2 counterparts, which mainly attributed to their abundant oxygen vacancies and stronger Ni–TiO2 interaction. In addition, both the narrower band gap and higher light absorption ability directly promoted the Ni/TiO2 catalyst possessing outstanding ethanol conversion (94.5%) and controllable H2/CO ratio (0.65) at 450 °C. Furthermore, the relatively less activation energy also determined that the Ni/TiO2 sample possessed the fastest kinetic progression in the EDR process. Therefore, the Ni/TiO2 catalyst exhibited the better photothermal catalytic activity compared with other 2 samples. We anticipate that photothermal synergy would offer good technical guidance to promote the conversion and utilization of greenhouse gas CO2 under relatively low temperature environment.
研究领域:
环境科学
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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
PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
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2022
·
IF 7.926
Wei Li,Xuesen Du,Zhi Li,Yaqin Tao,Jingyu Xue,Yanrong Chen,Zhongqing Yang,Jingyu Ran,Vladislav Rac,Vesna Rakić
Vanadia-based catalysts are widely used in selective catalytic reduction (SCR) reaction for reducing nitrogen oxides emissions, however, they only exhibit sufficient DeNO x efficiency within a narrow temperature window. In this study, a catalyst embedded with electrothermal alloy was prepared. The catalyst surface temperature could be heated using the electrothermal alloy, in order to widen the operating temperature window of the V 2 O 5 -WO 3 /TiO 2 catalyst. Experimental results revealed that the electrothermal alloy embedded V 2 O 5 -WO 3 /TiO 2 catalyst can maintain superior NH 3 -SCR performance and high resistance to H 2 O in a wide gas temperature range of 100–400 °C by controlling the surface temperature. In the meantime, the NH 4 HSO 4 poisoned catalyst could be efficiently regenerated through electric heating, and NO x conversion can be restored to the level of fresh samples. Additionally, the effect of additives including methylcellulose and glass fiber , on the physicochemical properties of the plate-type catalyst was also investigated, and the catalyst samples were characterized by means of BET, XRD , NH 3 -TPD, H 2 -TPR, TG and SEM-EDS. This study proves the electric heating strategy is a promising way to enhance the performance of the V 2 O 5 -WO 3 /TiO 2 during wide temperature SCR applications.
研究领域:
环境科学
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催化化学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2022
·
IF 4.889
Yaping Zhang,Guobo Li,Peng Wu,Hongqiang Yang,Sheng Wang,Kai Shen,Ling Wang
TiO 2 -Vo support with abundant oxygen vacancy was prepared by hydrothermal method, purchased TiO 2 -P for comparison, and Pd 0.12 V 4 /TiO 2 catalysts with different TiO 2 structures were prepared to investigate catalytic oxidation for dichloromethane (DCM). Pd 0.12 V 4 /TiO 2 -Vo catalyst showed excellent low temperature DCM removal efficiency, T 90 of which reduced to 290 ℃, and Cl resistance was maintained in 40 h. Abundant oxygen vacancy of TiO 2 -Vo was formed in transformation process of part anatase TiO 2 to rutile phase. The obtained Pd 0.12 V 4 /TiO 2 -Vo catalyst possessed rich acid sites, higher adsorbed oxygen (O ads ) ratio and better oxygen mobility, which inhibited loss of active components and improved DCM removal efficiency. DCM removal efficiency of Pd 0.12 V 4 /TiO 2 catalyst was reduced by HCl, while negative effect in the way of weakening competitive adsorption between HCl and DCM, that would be reduced by TiO 2 supports modification. The present work is favorable for further DCM removal catalyst anti-Cl poisoning modification and application in manufacture industry.
研究领域:
环境科学
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材料科学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2018
·
IF 4.521
Li Cao,Lei Chen,Xiaodong Wu,Rui Ran,Tengfei Xu,Ze Chen,Duan Weng
The CeO 2 /TiO 2 catalyst was prepared by a deposition-precipitation method, which exhibited high low-temperature activity under the fast SCR condition. By using transient reaction analysis (TRA), the steps in the fast SCR, including NO 2 adsorption and decomposition, reaction between nitrates and NO, ammonium nitrate formation and reduction by NO, were investigated. Diffuses reflectance infrared Fourier transform spectroscopy (DRIFTS) experiments, via NO + O 2 or NO + NO 2 adsorption, ammonium species reaction with NO x and NO reaction with NH 4 NO 3 , were designed to identify the roles of NO, NO 2 and NH 3 in fast SCR. Based on L-H mechanism, the NH 4 NO 3 formation played an important role in low-temperature SCR reaction. Compared with the behavior in standard SCR, the higher activity in the presence of NO 2 was ascribed to the faster NH 4 NO 3 formation rate and larger amounts of nitrates/nitrites. This phenomenon provided a basis for developing Ce-based catalysts as SCR catalysts for diesel exhaust aftertreatment.
研究领域:
催化化学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
ChemCatChem
·
2019
·Vol. 11
·期 16
·3919-3926
·
IF 4.495
Ke Liu,Zhenbo Zhao,Weiwei Lin,Qiang Liu,Qifan Wu,Ruhui Shi,Chao Zhang,Haiyang Cheng,Masahiko Arai,Fengyu Zhao
Graphical Another drop of copper : A non-noble metal catalyst of Cu/TiO 2 is effective for the heterogeneous N -methylation of N -methylaniline with CO 2 and H 2 , in which CHO* is formed as methyl reagent, and it reacts with N -methylaniline to produce intermediate N -methylformanilide followed by its hydrogenation to N,N -dimethylaniline. A non-noble heterogeneous catalyst of Cu/TiO 2 was prepared for N -methylation of N -methylaniline (MA) with CO 2 and H 2 . 5 wt.–% Cu loaded TiO 2 (P25) catalyst exhibited a high performance, with 82 % MA conversion and 98 % N,N -dimethylaniline (DMA) selectivity under the reaction conditions used (4 MPa H 2 , 2 MPa CO 2 , 180 °C, 36 h). The Cu/TiO 2 catalyst was more effective with respective to the total conversion and the DMA selectivity as compared to 5 wt.–% Cu loaded catalysts on CeO 2 , ZnO and activated carbon materials. The possible active species of Cu/TiO 2 catalyst should be both Cu + and Cu 0 which contributed to the high activity as the reaction conversion increased linearly with them exposed on the surface of catalyst. Moreover, the reaction pathways involved were studied; it was likely that the reaction took place via an intermediate of formaldehyde that was formed from CO 2 and H 2 , as confirmed by in situ diffuse reflectance Fourier-transform infrared spectroscopy, then it reacted with MA to give N -methylformanilide (MFA), and finally MFA was hydrogenated to DMA.
研究领域:
催化化学
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环境化学
✓ 已验证
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2018
·
IF 6.653
Yawei Feng,Hao Li,Lili Ling,Sa Yan,Donglai Pan,Hao Ge,Hexing Li,Zhenfeng Bian
The introduction of a piezoelectric field has been proven a promising method to enhance photocatalytic activity by preventing photoelectron–hole recombination. However, the formation of a piezoelectric field requires additional mechanical force or high-frequency ultrasonic baths, which limits its potential application on industrial scale. Therefore, it is of great practical significance to design the catalyst that can harvest the discrete energy such as the fluid mechanical energy to form the electric field. Herein, PZT/TiO2 catalyst with a core–shell configuration was prepared by a simple coating method. By collecting the mechanical energy of water, an internal piezoelectric field was induced. Under 800 rpm stirring, transient photocurrent measured on PZT/TiO2 electrode is about 1.7 times higher than that of 400 rpm. Correspondingly, the photocatalytic degradation rate and mineralization efficiency of RhB, BPA, phenol, p-chlorophenol much improved, showing the promoting effect of piezoelectric field generated directly from harvesting the discrete fluid mechanical energy.
研究领域:
材料科学
·
环境科学
✓ 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）