Journal of Materials Chemistry A
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2020
·Vol. 8
·期 19
·9813-9824
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IF 11.301
Yue Li,Jian Song,Mengting Jiang,Mbage Bawa,Xiaohong Wang,Yuyang Tian,Guangshan Zhu
Na5[IMo6O24]·3H2O and a porous aromatic framework (iPAF-1) were used to build an off-the-shelf building material (IMo6@iPAF-1) to realize the highly efficient oxidation of organic sulfurs like oxygenase. The synergy between IMo6 and iPAF-1 resulted in a higher BET surface area, hydrophobic microenvironment, and redox sites to show higher activity in aerobic oxidative desulfurization with almost 100% removal of model organic sulfurs under atmospheric pressure with almost 246 times higher TOFs compared to IMo6. It also showed efficiency in the desulfurization of gasoline and diesel to give very low S contents of 7.1 and 7.6 ppm with 99.3% and 99.4% removal, respectively, at 100 °C for 6 h. More importantly, IMo6@iPAF-1 could also catalyze desulfurization using concentrated O2 mixed with N2 or air instead of pure O2 with better safety and economics, while as low as 4.9 and 6.9 ppm S contents were achieved for gasoline and diesel, respectively. The special surroundings of IMo6@iPAF-1 repelled the sulfone product and allowed it to perform with the same efficiency when recycled without any treatment of the used catalyst.
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JOURNAL OF HAZARDOUS MATERIALS
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2020
·
IF 9.038
Yong Liu,Ni Tan,Jinrui Guo,Jianlong Wang
In this study, a novel Al°-CNTs-Cu 2 O composite, capable of activating O 2 to generate H 2 O 2 and further to reactive oxygen species (ROSs) at a wide pH range, was synthetized, characterized and applied for the degradation of sulfamerazine. In the activation of O 2 by Al°-CNTs-Cu 2 O composite, H 2 O 2 was generated from the reaction of O 2 with Al°-CNTs, which could be catalytically decomposed into O 2 − and OH by Cu 2 O, the formed Cu(II) could be rapidly reduced to Cu 2 O by Al°-CNTs in composite, which made Al°-CNTs-Cu 2 O composite reusable and decreased the leaching of copper ions into solution. The removal efficiency of SMR and TOC was 73.91 % and 56.80 %, respectively at initial pH = 5.8, T = 20 °C, O 2 flow rate = 100 mL/min, Al°-CNTs-Cu 2 O dosage = 2 g/L, SMR = 50 mg/L, and reaction time = 60 min. The removal efficiency of SMR kept almost unchanged and the concentration of copper ions in solution was below 0.5 mg/L. The Al°-CNTs-Cu 2 O/O 2 process could be used as a novel catalyst for the degradation of refractory organic contaminants in water and wastewater by Fenton-like process at a wide pH range through the in situ generation of H 2 O 2 .
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NEW JOURNAL OF CHEMISTRY
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2020
·Vol. 44
·期 27
·11808-11816
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IF 3.288
Shi-Yuan Zhang,Jing-Jing Ma,Hong-Lin Zhu,Yue-Qing Zheng
Syngas, as a necessary feedstock dependent on non-renewable fossil fuels, is a mixture of CO and H2, which could be prepared by a renewable strategy via electrochemical CO2 reduction in water electrolyte solutions. Herein, beaded Au@Co3O4 nanowire arrays (denoted as Au@Co3O4 NAs) were obtained by immersion in HAuCl4 solution with Co3O4 nanowire arrays. The Au@Co3O4 NAs exhibited outstanding electrochemical performance of producing syngas via tuning from 1 : 1 to 4 : 1 with controlling voltage. In addition, the Au@Co3O4 NAs showed better catalytic performance for the oxygen evolution reaction with an overpotential of 320 mV at a current density of 50 mA cm−2, along with a small Tafel slope of 75 mV dec−1 in 1 M KOH solution. The electrochemical performance of Au@Co3O4 NAs is obviously superior to Co3O4 NAs, which will open up a viable strategy for the design and fabrication of a bi-functional electrocatalyst for the overall reaction (CO2 + H2O → CO + H2 + O2).
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yu Luo,Chenchen Liu,Jiahui Liu,Xueming Liu,Yang Zhou,Xinwen Ou,Bo Weng,Jin Jiang,Bin Han
Photocatalytic O 2 reduction presents a sustainable strategy for H 2 O 2 synthesis, while the in-situ decomposition of H 2 O 2 significantly deteriorates the activity and stability. Here, by introducing anthraquinone centers into covalent organic frameworks (DQTb-COFs), for the first time, we realized the suppression of in-site decomposition of generated H 2 O 2 via site-engineering of COFs. Under visible light irradiation, DQTb-COFs achieves an H 2 O 2 generation rate of 1844.1 μmol h −1 g −1 without sacrificial agents, which is about 3.4 times that of its counterpart without anthraquinone centers (DATb-COFs). The generated H 2 O 2 on DATb-COFs is readily reduced into hydroxyl radicals (•OH), which is not observable on DQTb-COFs. Experiments and calculations demonstrated that the anthraquinone centers of DQTb-COFs can enhance the generation of H 2 O 2 by facilitating the utilization of O 2 and promoting the desorption of H 2 O 2 . This work highlights how to inhibit the in-situ decomposition of H 2 O 2 via site-engineering of COFs, and blazes a new trail for highly efficient H 2 O 2 photosynthesis.
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Journal of Materials Chemistry A
·
2015
·Vol. 4
·期 4
·1399-1407
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IF 7.443
Guangyu Zhao,Li Zhang,Jixian Lv,Changle Li,Kening Sun
Hydrothermal self-assembly is a highly efficient and low cost method to prepare graphitic foam from graphene oxides; however, the self-assembly frameworks usually do not have controllable pore structures because of the spontaneous process. In this paper, a hydrothermal synthesis assisted by ammonium peroxo-polymolybdate [(NH4)2Mo2O11] tailoring to fabricate graphitic foam is presented. The foam possesses pore structures which can be controlled by adjusting the rate of charge in the hydrothermal experiments. Furthermore, the foam obtained from a definite rate of charge [(NH4)2Mo2O11 : graphene oxide is 1 : 2 in weight] has a hierarchical pore structure and a through-hole net. In electrochemical energy storage, such unique features are beneficial for providing efficient mass transport as well as abundant, accessible active sites. The graphitic foam was tested for use as self-supported electrodes of Li–O2 batteries (LOBs) and Li ion batteries (LIBs) without any metallic current collectors or organic binders, and the foam frameworks exhibited remarkable lithium ion storage properties in both of the two batteries (e.g., 5500 mA h g−1 at 0.2 A g−1 as LOB cathodes and 250 mA h g−1 at 50 A g−1 as LIB anodes).
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ACS Applied Nano Materials
·
2024
·
IF 5.3
Xiang Yu,Yuwei Mi,Zihan Gong,Yongfang Zhang,Lei Wang,Suyuan Zeng
Constructing heterojunctions is an effective strategy for increasing semiconductor photocatalytic activity. Herein, a Bi2O3/Bi4O5Br2 type-II heterojunction was synthesized using a simple one-pot solvothermal route. The 0-dimensional (0D) Bi2O3 nanoparticles are uniformly distributed within the 2D Bi4O5Br2 nanosheets with (101̅) facets dominantly exposed. In comparison with pure Bi2O3 and Bi4O5Br2, they show higher photocatalytic activity degradation of resorcinol (RO) and Rhodamine B (RhB). The Bi2O3/Bi4O5Br2 composite containing 10% Bi2O3 (BOB4) displays the best photocatalytic activity. For instance, compared with pure Bi4O5Br2 and Bi2O3, the k(RO) values of BOB4 (0.58 h–1) are 3.1 and 4.8 times higher. The enhanced photocatalytic activity is attributed to the formation of a large heterojunction interface that results from the homogeneous distribution of Bi2O3 nanoparticles in the Bi4O5Br2 nanosheet, which effectively enhances the photogenerated charge separation in a type-II mode. Major active species include superoxide radicals (•O2–), hydroxyl radicals (•OH), and holes (h+). In addition, the Bi2O3/Bi4O5Br2 photocatalysts exhibit outstanding resistance to inorganic ions, pH, water matrix, as well as outdoor sunlight and favorable stability and biocompatibility. This work presents a simple method to construct Bi-based heterojunction architectures for photoactivity improvement.
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CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Wei Du,Zhihua Zhang,Jundi Wang,Nan Song,Xuezhi Duan,Xinggui Zhou
Propylene epoxidation by H 2 and O 2 to propylene oxide (HOPO), as a novel method for PO production, has attracted widespread attention due to its economic and environmental advantages. Acrolein is a notable byproduct arising in HOPO reaction over Au/TS-1 catalyst, and is traditionally thought to be exclusively formed on Au site through propylene oxidation. However, on the intraporous and external surface Au sites of Au-Ti catalysts, the HOPO reaction have been shown to proceed by different mechanisms, yet the effect of active sites distribution on acrolein formation is far from being understood. Herein, we found that the reaction orders in acrolein formation on Au/TS-1 catalyst (H 2 , 0.19; O 2 , 0.44; C 3 H 6 , 0.44) relative to Au/TS-1 with blocked pores (Au/TS-1-B) catalyst (H 2 , −0.36; O 2 , 0.61; C 3 H 6 , 0.52) were quite different, suggesting a variation in the reaction pathway on the catalysts with different Au locations. Moreover, it is found that PO can be converted to acrolein by O 2 on TS-1 zeolite, which is absent on TS-1-B zeolite without micropores. Consequently, acrolein formation on Au/TS-1 catalyst can proceed through two parallel pathways: propylene hydro-oxidation on Au site, and PO conversion by O 2 inside micropores. Furthermore, by designing and preparing the Au/TS-1 catalysts with different structures, the Au locations are closely related to acrolein formation mechanism and kinetic behaviors. This work provides kinetic insights into the acrolein formation pathways in the HOPO reaction on Au/TS-1 catalyst, and is helpful to the rational design and preparation of efficient catalysts with high selectivity.
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Chemical Science
·
2024
·
IF 7.6
Yinglei Tao,Tao Wang,Xingyu Yu,Ke Gong,Hao Gong,Haixia Chen,Xiaoli Fan,Aidi Zhang,Xianli Huang,Kun Chang,Jianping He
Li–O2 batteries (LOBs) boast an exceptionally high theoretical energy density; however, the slow kinetics of the oxygen electrode reaction have been a significant hurdle in their advancement and practical application. In this study, a composite of bismuth oxyhalide heterojunction incorporated with metal–organic frameworks (MOFs) was engineered on carbon cloth (Zr-MOF/BiOIBr/CC) as an efficient bifunctional catalyst to enhance the oxygen electrode reaction in photo-assisted LOBs. Compared to Zr-MOF/CC, Zr-MOF/BiOIBr/CC significantly expands the light absorption spectrum of the catalyst. Furthermore, the built-in electric field in the heterojunction aids in the separation and directional movement of photogenerated carriers, thereby expediting the reaction kinetics of LOBs. Consequently, the photo-assisted LOBs with Zr-MOF/BiOIBr/CC as the cathodes display a discharge potential of 3.05 V, a low charge potential of 3.20 V, and an energy efficiency of up to 95.3%, and can sustain an extended cycle life of over 255 cycles. This study underscores the potential application of MOFs/semiconductor heterostructural materials in photo-assisted LOBs and offers insights into the systematic design of photo-assisted air batteries and other advanced semiconductors.
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CATALYSIS TODAY
·
2024
·
IF 5.2
Jipeng Wang,Xinli Tong,Chen Guo,Yahui Wei
The high entropy oxides are widely studied as the potential catalytic materials owing to their unique structure and excellent properties. In this work, a new high entropy oxide catalyst MnFeCoNiCuO x was successfully prepared and used for the oxidative condensation reaction of furfural (FUR) and aliphatic alcohol , where the carbon-chain length can be selectively increased under the mild conditions. For the selective oxidative transformation of FUR with n-butanol, a more than 99.0 % conversion of FUR and 91.5 % selectivity of 2-(furanyl-2-methylene) butanal was obtained at 80 ºC for 2 h. In addition, the oxidative condensation of FUR with ethanol, n-propanol, n-pentanol, n-hexanol and n-heptanol was also carried out with the MnFeCoNiCuO x - LiOH as catalyst system in the presence of molecular oxygen , where a moderate to high product yields were acquired. Furthermore, the characterizations of catalyst showed that the existence of abundant oxygen vacancy and high specific area was greatly important to the catalytic reactions .
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Yajuan Jiang,Shining Zhang,Chunyu Xu,Bin Jia,Shijie Ren,Wenyu Zheng,Yicong Huang,Kunpeng Jiang,Xiuyun Zhang,Yunyun Zhao,Guisheng Zhu,Huarui Xu
In this paper, biomass carbon@Li(Ni 0.6 Co 0.4 )O 2 (BC@LNCO) micron-tube is successfully synthesized via a bio-templating method as cathodic material for lithium-ion hybrid supercapacitors. Cobalt nickel subcarbonates nanowires arrays are homogeneously grown on bagasse substrate via a unique synthesis strategy using a toluene-water interface reaction process, which subsequently transform as BC@LNCO micron-tube after lithiation process. The distinctive biomass fibre structure of bagasse biomass carbon leads to a significant enhancement in active sites in the BC@LNCO composite, which facilitates lithium-ion diffusion and enhances the contact area between the electrode and electrolyte. So, the prepared BC@LNCO electrode demonstrates improved electrical performances with a high specific capacitance of 921 F g −1 at 1 A g −1 and a good rate performance with 72 % retention at 10 A g −1 . In addition, the lithium-ion hybrid supercapacitor is fabricated with BC@LNCO and activated carbon (AC) as positive and negative electrodes, respectively. The BC@LNCO//AC device demonstrates a good energy density of 56.25 Wh kg −1 at 818.4 W kg −1 , and maintains 25.06 Wh kg −1 when the power density is up to 8143.42 W kg −1 , indicating that the prepared BC@LNCO composite can be a promising candidate as electrode material for Li-ion hybrid supercapacitor.
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PROCEEDINGS OF THE COMBUSTION INSTITUTE
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2024
·
IF 5.3
Nan Liu,Qi Chen,Xianwu Jiang,Jie Chen,Lidong Zhang,Jiaying Pan,Haiqiao Wei,Xingqian Mao
This work presents a three-stage hybrid nanosecond discharge (NSD) and direct current (DC) discharge assisted n -C 5 H 12 /O 2 /N 2 ignition with lower discharge energy and higher energy efficiency. The reaction rate coefficients between O 2 (a 1 Δ g ) and n -C 5 H 12 are updated by mass/Master equation simulation. The promotive ignition enhancement via reaction channel O 2 (a 1 Δ g ) + n -C 5 H 12 → C 5 H 10 + H 2 O 2 in the hybrid NSD/DC discharge is demonstrated. The results show that the ignition delay time of the three-stage hybrid plasma assisted ignition is 1–2 orders of magnitude shorter than that of the two-stage hybrid discharge when the reduced electric field strength in the DC discharge stage is over 10 Td. Meanwhile, the plasma-enhanced energy efficiency of three-stage hybrid discharge increases. This improved efficiency on ignition enhancement is due to the kinetic enhancement by the electronically excited species and radicals (O 2 (a 1 Δ g ), O( 1 D), N 2 (B) and O). The kinetic and thermal effects by plasma are effectively intergated to enhance ignition. However, more discharge energy deposited in the vibrationally excited states N 2 ( v ) in the two-stage hybrid discharge is less efficient on ignition enhancement due to the thermal contribution via vibrational-translational relaxation. In the aspect of NO x /N 2 O emissions, reduction efficiency of the three-stage hybrid discharge is two times higher than that of the two-stage hybrid discharge. By controlling the N/N( 2 D) production pathway e + N 2 → e + N + N( 2 D), the three-stage hybrid discharge reduces NO x and N 2 O production by 61.1 % and 90 %, respectively. The results show that the ignition delay time is non-monotonically dependent on the discharge pulse number. There exist optimal pulse number, reduced electric field and effective threshold power density of DC discharge to achieve maximum ignition enhancement and low NO x /N 2 O emissions. This study provides valuable insights into the use of NSD/DC hybrid discharge technology in advanced engines to achieve energy-efficient ignition enhancement and reduce NO x /N 2 O emissions.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Yixi Wang,Wenqing Xu,Zhi Liu,Yulong Shan,Wanrong Chen,Xinyu Zhang,Tingyu Zhu
Controlling both CO and NOx pollutants without additional cost is necessary but challenging, especially in industrial flue gas with complex components. Previous studies mainly focused on the effect of O 2 and SO 2 on the CO oxidation side reaction and valence state of Ir species on various catalysts, while neglecting the impact on NO conversion pathway. Herein, we propose an "ineffective reaction pathway" in the presence of O 2 with nitrate as an intermediate according to the results of in situ DRIFTS and DFT. And we also reveal the contribution of SO 2 in inhibiting the adsorption of O 2 and promoting the selective adsorption of NO and CO even at lower injection concentrations, based on the oxidation of SO 2 on Ir(111). This is quite a favorable characteristic for the treatment of industrial flue gas, resolving the long–standing dispute on the involvement of these components in the CO–SCR reaction. Under specific conditions (CO/NO=20, O 2 =5%, SO 2 =200 ppm) at 250 °C, the NOx conversion is as high as 78%. These results will contribute to the development of more efficient catalysts in the future for simultaneously controlling two pollutants (CO and NOx).
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