PROCEEDINGS OF THE COMBUSTION INSTITUTE
·
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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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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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2025
·
IF 11.3
Jingwen Qian,Mingyi Yu,Zheng Lian,Shule Zhang,Qin Zhong
An innovative strategy in wet flue gas denitration technology was proposed to control nitrogen oxide emissions from cement kiln. Here the use of tetrabutylammonium bromide (TBAB) as an additive improved the absorption and utilization efficiency of sulfite absorbents for NO2. Compared with the sulfite solution, the stability time and absorption efficiency of adding TBAB were increased from 25 to 76 min and from 91.2 to 98.4%, respectively. Continuous absorption for 480 min indicated the feasibility of TBAB for repeated use. Moreover, we propose an antioxidant mechanism, including the capture of SO3•– by TBA+, and the reduction of SO3•– by Br–. The successive steps kept the sulfite from the cyclic depletion of the radical chain reaction of “Generate SO3•–-Introducing O2–Consuming SO32–” due to O2. A new application of TBAB in free radical trapping and antioxidant is given. Furthermore, a kinetic model describing the macroscopic absorption rate was developed based on different operating conditions.
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ACS Applied Materials & Interfaces
·
2025
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IF 8.2
Yingnan Zhu,Jiahang Si,Tiantian Xu,Lan Zheng,Xinyu Xiao,Xiaohan Sun,He Ding,Yuze Dong
Chemodynamic therapy (CDT) and photodynamic therapy (PDT) have emerged as promising strategies for treating skin abscesses. However, their therapeutic efficacy is fundamentally constrained by the hypoxic and hydrogen peroxide-deficient microenvironment characteristic of abscesses. Herein, we developed a near-infrared (NIR) light-responsive nanoplatform (ICG/CuO2@PCM) by encapsulating copper peroxide (CuO2) and indocyanine green (ICG) within a phase-change material (PCM), which enables control over self-supplied H2O2/O2 release via an NIR-triggered cascade. Upon irradiation, ICG-mediated photothermal conversion elevates the temperature beyond the PCM melting threshold, triggering a burst release of CuO2 and ICG. CuO2 generates hydroxyl radicals (•OH) through a Fenton-like reaction in the acidic wound microenvironment. Additionally, CuO2 can thermally decompose under photothermal conditions to produce a sustained oxygen supply, which ICG immediately converts into singlet oxygen (1O2), thereby enhancing PDT efficiency. Furthermore, photothermal therapy not only enhances the efficiency of CDT but also provides additional antibacterial support. Remarkably, ICG/CuO2@PCM (NPs), coupled with irradiation, accelerate abscess wound recovery by dispersing biofilm, killing bacteria, and promoting macrophage polarization toward an anti-inflammatory phenotype. Overall, this NIR-responsive nanoplatform highlights the promise in controlled modulation of microenvironment-adaptive antimicrobial strategies to overcome current limitations of hypoxic infections.
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Energy Materials
·
2025
·Vol. 5
·期 11
·N
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IF 11.2
Shukai Liu,Huang Tan,Gaole Dai,Shiyun Xiong,Yu Zhao,Benxia Li
The oxygen evolution reaction (OER), as a pivotal process in electrochemical water splitting, directly determines energy conversion efficiency. Ruthenium (Ru)-based catalysts have gained considerable attention in recent years due to their decent intrinsic activity in acidic media. Previous studies have demonstrated that while Ru exhibits superior OER activity compared to RuO2 in acidic environments, its operational stability remains markedly inferior. This performance dichotomy, coupled with the persistent challenges of active species dissolution and catalyst particle aggregation during prolonged operation, significantly hinders their practical implementation in electrochemical systems. To address these challenges, this study develops a carbon nanotube (CNT)/Fe-Ni@RuO2@PANI-350 composite catalyst composed of RuO2 nanoparticles supported on bimetallic Fe-Ni modified CNTs (CNT/Fe-Ni) and encapsulated with polyaniline (PANI). This catalyst utilizes the anchoring effect of bimetallic Fe-Ni sites and the spatial confinement effect of PANI coating layer, effectively inhibiting the dissolution and agglomeration of RuO2 during both high-temperature processing and electrochemical operation, thereby significantly enhancing electrochemical stability. The anchoring strength of RuO2 nanoparticles on CNT/Fe-Ni support via the nano-confinement effect, as well as the microscopic mechanisms underlying the performance enhancement, are revealed by density functional theory calculations and experimental characterizations. The composite catalyst demonstrates fascinating OER performance in 0.5 M H2SO4, exhibiting a low Tafel slope of 39.1 mV dec-1 as well as low overpotentials of 188 and 225 mV at current densities of 10 and 100 mA cm-2, respectively. Remarkably, the composite catalyst demonstrates significantly enhanced stability, exhibiting only ~30 mV overpotential increase during 150 h continuous operation at 10 mA cm-2. This study highlights a simple yet effective nano-confinement strategy to address the challenges of Ru-based catalysts, and provides a practical paradigm for designing and preparing highly efficient OER electrocatalysts with enhanced stability.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
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IF 9
Cailiang Yue,Yukun Tian,Linlin Zhu,Nan Sun,Zhiqi Zhou,Fuqiang Liu,Yifei Sun
Photocatalytic 1 O 2 generation has emerged as a promising technology for environmental remediation and organics synthesis. Nevertheless, the efficiency of photocatalytic 1 O 2 generation via O 2 activation through charge-transfer mechanism remains challenging in carbon nitride due to the weak dielectric screening effect. Herein, series of uric acid (UA)-modified ultrathin carbon nitride nanosheets (UCN-x) were fabricated by the simple supramolecular self-assembly process. Comprehensive characterizations revealed that the incorporation of UA pigment would induce purine structure into heptazine skeleton. Photocatalytic experiments showed that the modification of UA greatly enhanced photocatalytic 1 O 2 generation ability. The optimal UCN-2 exhibited superior photocatalytic degradation of tetracycline (TC) with the normalized TC degradation rate up to 10.03 mg TC g cat −1 min −1 , which was 2.1–31.1 times as high as that of reported photocatalysts. What's more, UCN-2 exhibited excellent photocatalytic TC degradation across diverse aqueous conditions, demonstrating significant potential in environmental remediation. Time-dependent density functional theory (TD-DFT) calculation revealed that the doping of UA could trigger the spatial separation of h + /e − distribution, with h + concentrated in UA pigment and e − concentrated in adjacent heptazine ring. The engineered adjacent redox sites were precisely tailored to align with the charge-transfer mechanism for photocatalytic 1 O 2 generation. This work established a fundamental framework for designing highly efficient photocatalysts with manipulated O 2 activation.
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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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Joule
·
2022
·
IF 46.048
Qing Han,Wei Guo,Xiaofeng He,Tongchao Liu,Xiao Liu,Xuebing Zhu,Tengfei Bian,Lei Jiang,Jun Lu,Yong Zhao
Aprotic lithium-oxygen (Li-O 2 ) batteries have attracted extensive attention due to their ultrahigh theoretical energy density. However, slow and undesired electron transfer during cathodic reactions causes low cyclic stability in these batteries. Here, we demonstrate that O 2 mass transport and electron transfer for cathodic reactions in Li-O 2 batteries could be decoupled by a double-cathode structure that efficiently enables stable electron transfer between the cathode and Li 2 O 2 /O 2 . This resolves various side reactions and slow Li 2 O 2 reaction kinetics issues in conventional Li-O 2 batteries, leading to stable operation of the cell for nearly 2 months at a capacity of 0.2 and 5 mAh cm −2 , with more than 4- and 10-fold increases in cycle life when compared with single-cathode batteries. These remarkable improvements in the cyclic stability of Li-O 2 batteries with double cathodes provide an interesting concept for improving the operational stability of other metal-rechargeable batteries with conversion-type chemistry.
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Science Bulletin
·
2025
·
IF 21.1
Ergui Luo,Jingyi Liang,Kexuan Zhang,Xian Wang,Luozhen Jiang,Tianjun Hu,Junming Zhang,Junjie Ge,Jianfeng Jia
Electrochemical two-electron oxygen reduction reaction (2e − ORR) serves as an appealing approach for green hydrogen peroxide (H 2 O 2 ) production. However, the corresponding progress in efficient non-precious metal catalysts for acidic 2e − ORR has not kept pace, with the research model being almost confined to Co-based system. Here, guided by molecular dynamics simulations, the active nature and origin of pyrolyzed Cr−N 4 catalysts for ORR are unveiled, wherein the over-strong oxygen affinity of the Cr center is counterbalanced by a spontaneous axial O-coordination. By creating an oxidation-induced electron-deficient environment, the Cr−N 4 can be flexibly tailored for selective H 2 O 2 formation. A single-atom Cr−N 4 /C(O) catalyst is developed experimentally, which rivals and even slightly outperforms its Co-based counterpart in terms of selectivity (92% versus 71%) and productivity (202 versus 145 mmol g cat −1 h −1 ) for H 2 O 2 . More encouragingly, the Cr-based catalysts exhibit minimal reactivity towards H 2 O 2 -related side reactions, with the metal component being robust against leaching. This research marks the first identification of pyrolyzed Cr−N 4 catalysts as competent for acidic two-electron O 2 reduction to H 2 O 2 . The innovative models and insights offer profound guidance for the design of future-generation catalysts for electrochemical H 2 O 2 synthesis.
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ADVANCED FUNCTIONAL MATERIALS
·
2021
·Vol. 32
·期 15
·2111125
·
IF 18.808
Binyao Liu,Jinyan Du,Gaili Ke,Bi Jia,Yujie Huang,Huichao He,Yong Zhou,Zhigang Zou
g -C 3 N 4 photocatalysis is a safe and green approach for H 2 O 2 production, but the activity of pristine g -C 3 N 4 photocatalysts is unsatisfactory. At present, most of the modifications on g -C 3 N 4 photocatalysts for H 2 O 2 production have focused on thermodynamic processes, few have considered the kinetic aspects. Herein, the surface N -hydroxymethylation of g -C 3 N 4 photocatalysts for the efficient kinetic production of H 2 O 2 is reported. Through the reaction of formaldehyde with the amino moieties (–NH 2 ) on the g -C 3 N 4 surface, N -hydroxymethyls groups (-NH-CH 2 -OH) are introduced on typical g -C 3 N 4 photocatalysts. Relative to the pristine g -C 3 N 4 photocatalysts, the modified g -C 3 N 4 photocatalysts have over 1280% higher activity for H 2 O 2 production in pure water system, and impressive solar-to-chemical conversion efficiency. The experimental investigations and theoretical calculations reveal that the introduction of -NH-CH 2 -OH on the g -C 3 N 4 photocatalysts does not change their morphology, light absorption intensity and edges, band positions, charge separation and transfer properties, but markedly improved the H 2 O dehydrogenation and O 2 adsorption properties of g -C 3 N 4 . As a result, the reduction kinetics of O 2 to H 2 O 2 on the g -C 3 N 4 photocatalysts with -NH-CH 2 -OH is more energetically favorable. This work provides a useful reference and inspiration to achieve the effective modification of g -C 3 N 4 or other metal-free photocatalysts from the kinetic perspective.
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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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