ACS Applied Energy Materials
·
2022
·
IF 6.959
Jie-wen Liu,Jian Zhang,Ming-jie Xu,Chuan-jin Tian,Xiao-jun Zeng,Chang-an Wang
Developing highly active and reliable Pt-based catalysts is a major challenge for the widespread commercialization of proton-exchange membrane fuel cells. Herein, we have designed Pt3Co@C hollow sphere catalysts by the template method, in which PtCo alloy nanoparticles of approximately 3 nm diameter are anchored in a porous shell of nitrogen-doped carbon hollow spheres. Due to the confinement effect of the porous carbon shell, PtCo alloy nanoparticles possess excellent resistance to sintering, maintaining 2–3 nm size after calcination at 800 °C. Also, Pt3Co@C hollow sphere catalysts exhibit superior catalytic activity and stability in the oxygen reduction reaction, achieving 3.6 times the mass activity of the corresponding commercial Pt/C catalyst. Such catalysts with a mass activity retention rate of 87% after accelerated durability testing and no significant decay in activity after 10,000 potential cycles. Meanwhile, Pt3Co@C catalysts exhibit extremely high catalytic activity and surprising durability for the hydrogen evolution reaction process over the entire pH range. We believe that this methodology provides an insight into the preparation of high-performance electrocatalysts.
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ENVIRONMENTAL RESEARCH
·
2022
·
IF 8.431
Yong Cheng,Han-Qing Zhao,Aqiang Ding,Fei Chen,Jun Liu,Dazhi Fang,Chenglong Li,Yongkui Huang,Peili Lu
The widespread application of quaternary ammonium compounds (QAC) has posed a serious hazard to the environment and human being, and high concentration of Cl − in QAC wastewater may further increase the difficulty of pollutants elimination . In this study, such a QAC wastewater under high salinity conditions was chosen as the target, the prepared Ti/(Ru x Ir y )O 2 anode exhibited favorable catalytic performance for the oxidation and mineralization of QAC under high salinity conditions. Increasing the Ru/Ir ratio of Ti-based electrode coating also slightly promoted the inner catalytic capacity. The combination of electron paramagnetic resonance (EPR) and quenching experiments indicates that 1 O 2 served as a main reactive specie in the Ti/(Ru x Ir y )O 2 electrooxidation system. The increase of pH could decrease the removal efficiency of QAC for the reduced 1 O 2 yield, and the rise of Cl − concentration could favor the QAC oxidation, and Cl − was a better electrolyte to promote the oxidation of organic contaminants when compared to Na 2 SO 4 or Na 2 CO 3 . Additionally, the conversion pathway of the model pollutant was tentatively investigated, the results demonstrated that there were almost no halogenated final products residual by electrocatalytic oxidation with Ti/(Ru x Ir y )O 2 anode. This study not only elucidate the reaction mechanism of Ti/(Ru x Ir y )O 2 anode electrocatalytic oxidation of high salinity QAC wastewater, but also may provide an efficacious and eco-friendly method for the treatment of high salinity QAC wastewater.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2021
·
IF 9.028
Liying Wu,Zhiqiang Sun,Yufei Zhen,Shishu Zhu,Chen Yang,Jing Lu,Yu Tian,Dan Zhong,Jun Ma
Ubiquitous oxygen vacancies (Vo) existing in metallic compounds can activate peroxymonosulfate (PMS) for water treatment. However, under environmental conditions, especially oxygenated surroundings, the interactions between Vo and PMS as well as the organics degradation mechanism are still ambiguous. In this study, we provide a novel insight into the PMS activation mechanism over Vo-containing Fe–Co layered double hydroxide (LDH). Experimental results show that Vo/PMS is capable of selective degradation of organics via a single-electron-transfer nonradical pathway. Moreover, O2 is firstly demonstrated as the most critical trigger in this system. Mechanistic studies reveal that, with abundant electrons confined in the vacant electron orbitals of Vo, O2 is thermodynamically enabled to capture electrons from Vo to form O2•– under the imprinting effect and start the activation process. Simultaneously, Vo becomes electron-deficient and withdraws the electrons from organics to sustain the electrostatic balance and achieve organics degradation (32% for Bisphenol A without PMS). Different from conventional PMS activation, under the collaboration of kinetics and thermodynamics, PMS is endowed with the ability to donate electrons to Vo as a reductant other than an oxidant to form 1O2. In this case, 1O2 and O2•– act as the indispensable intermediate species to accelerate the circulation of O2 (as high as 14.3 mg/L) in the micro area around Vo, and promote this nano-confinement electron-recycling process with 67% improvement of Bisphenol A degradation. This study provides a brand-new perspective for the nonradical mechanism of PMS activation over Vo-containing metallic compounds in natural environments.
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Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 42
·24056-24063
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IF 12.732
Yanfang Chen,Xuemei Yan,Jixiang Xu,Lei Wang
H2O2 has a wide range of uses as an oxidant and is also utilized as a high density and environmentally friendly fuel. In this study, crystalline g-C3N4 was modified with K+, Ni and N-doped carbon by thermal-polymerization of Ni2+-anchored and polyvinyl pyrrolidone-encapsulated melamine-cyanuric acid supramolecules, followed by re-calcination in a KCl–LiCl mixture. The obtained strip-like g-C3N4 nanocrystals exhibited high charge separation efficiency and good light absorption capability. Density-functional theory calculations confirmed that the orbital hybridization of Ni–N atoms enabled the formation of charge-transfer channels, which can capture electrons, achieve enhanced oxygen adsorption and reduction via a two-electron pathway. Under the synergistic effects of K+, Ni and N-doped carbon dopants and crystallinity, the obtained sample exhibited high photocatalytic H2O2 yields of 79.6 μM in O2-saturated pure water, which was 10-fold higher than the yield using pristine g-C3N4. This work provides a novel design for production of highly efficient photocatalysts for H2O2 production.
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Nanoscale
·
2021
·Vol. 13
·期 16
·7774-7782
·
IF 7.79
Gangyong Li,Guangming Ren,Wei (Alex) Wang,Zongqian Hu
Carbonaceous materials are promising electrode materials for enzymatic biofuel cells (EBFCs) due to their excellent electrical conductivity, chemical and physical stability and biocompatibility. Design and preparation of carbon materials with a hollow structure and a rough surface are of great significance for immobilization of enzymes both inside and outside the carbon materials for EBFC applications. We report herein the synthesis of novel carbonaceous materials consisting of bamboo-shaped hollow N-doped carbon nanotubes (N-CNTs) and C3N4 nanosheets (denoted as N-CNTs@C3N4) as electrode materials for dual-capture of enzymes in glucose/O2 EBFCs. The combination of one-dimensional N-CNTs with an open structure and two-dimensional C3N4 nanosheets forms a three-dimensional crosslinking network that significantly enhances the immobilization of enzymes, electrode stability, and mass transfer of substrates, thus boosting the EBFC performance. As a result, EBFCs equipped with N-CNTs@C3N4 can generate a high open circuit potential of 0.93 V and output a maximum power density of 0.57 mW cm−2 at 0.47 V. Additionally, the as-fabricated glucose/O2 EBFCs are capable of directly harvesting energy from various soft drinks, which indicates the promising applications of the N-CNTs@C3N4 nanocomposite as an electrode material for EBFCs.
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Journal of Energy Storage
·
2022
·
IF 8.907
De-Ming Zhu,Fan Bai,Yi-Nan Zhang,Ya-Nan Yang,Zhuang Sun,Jun-Wen Deng,Tao Zhang
Solid-state Li-O 2 batteries (SSLOBs) have been denoted as the holy grail in next-generation Li metal batteries for their high theoretical energy density , manipulation of ambient air to energy storage as well as high safety. However, the solid rigid interfaces both at the cathode and anode side introduce ultra-high resistances in the battery system and impede its operation under ambient temperature. Moreover, the high-reductive Li anode and semi-open cathode would cause severe side reactions during cycling which further degrade battery performance. To manage the above-mentioned issues, a rationally designed SSLOBs based on plastic crystal electrolyte is proposed in this study to enable SSLOBs operation at ambient temperature and in full charge-discharge mode. The brand-new Li-O 2 battery has been improved mainly from two aspects. First, we propose a polyacrylonitrile (PAN) modified succinonitrile (SN) electrolyte (PAN-SN) to retard the polymerization of SN and meanwhile suppress the degradation of Li ionic conductivity. Second, we propose an alternative mixed electron/ion complex conductor (MEIC) cathode to coordinate with plastic crystal electrolyte with an expanded Li-O 2 reactive zone and improved interfacial charge transfer during the charge-discharge process. The fabricated flexible SSLOBs based on PAN-SN electrolyte and MEIC cathode could be successfully fully charged-discharged (cutoff 2.0–4.5 V) for tens of cycles at ambient temperature under simulated air condition (20 vol% oxygen), with high-capacity retention of around 85 %.
研究领域:
能源存储
·
电池技术
·
材料科学
·
电化学
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2018
·
IF 6.653
Yuan Chen,Xu Zhang,Shixiang Feng
Contributions of excited triplet state of humic acid (3HA*) and superoxide radical anion (O2•–), which is mainly generated via the reaction of O2 with HA-derived reducing intermediates (HA•–), to phenol transformation were revealed using acetaminophen, 2,4,6-trimethylphenol and tyrosine as probe molecules. Phenol transformation was initiated by 3HA*, leading to the formation of the phenoxyl radical (PhO•), but the distribution of transformation intermediates was codetermined by 3HA* and HA•–. The influence of HA•– essentially resulted from the production of O2•–, which affected the fate of PhO•. PhO• could undergo dimerization, or react with O2•–, leading to either phenol peroxide formation (radical addition) or phenol regeneration (electron transfer). In addition, PhO• could bind to HA or react with HA radicals, particularly in the absence of O2 and O2•–. These PhO• reactions were dependent on the reduction potential and structure of PhO•. This study also proved that the reaction of phenol with 1O2 and the reaction of PhO• with O2•– lead to the same oxidation product. The contributions of 3HA* and its generated 1O2, HA•– and its generated O2•– to phenol transformation were pH-dependent.
研究领域:
环境化学
·
物理化学
·
分析化学
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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.
研究领域:
材料科学
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环境科学
·
化学工程
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高影响因子
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 .
研究领域:
化学工程
·
催化科学
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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.
研究领域:
材料科学
·
能源存储
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Materials Today Energy
·
2022
·
IF 9.257
Jingjun Zhai,Haocheng Ji,Wenhai Ji,Rui Wang,Zhongyuan Huang,Tingting Yang,Chaoqi Wang,Taolve Zhang,Ziwei Chen,Wenguang Zhao,Akhil Tayal,Lei Jin,Jun Wang,Yinguo Xiao
Layered transition metal oxides have been broadly studied due to their great potential in application as cathodes for sodium-ion batteries. However, many single-phase layered transition metal oxides, especially those crystallized in P2- or O3-type structure, possess their individual characteristics incurring unsatisfactory overall performances with respect to the reversible capacity, rate capability, and cycling stability. Here, an effective strategy of constructing the P2/O3 biphasic structure is realized in layered cathode Na 0.7 Ni 0.4 Mn 0.4 Ti 0.2 O 2 through Ti substitution. Through high-resolution scanning transmission electron microscopy and X-ray diffraction, the formation of P2/O3 intergrowth structure was clarified and the proportion of the two phases was determined. Benefitting from the presence of intergrowth structure, the layered cathode provides a competitive rate capability of 100 mAh/g at a high rate of 5 C as well as a prominent cycling stability of 80.04% capacity retention after 300 cycles at 5 C. The improved performance is closely related to the highly reversible phase transition process from P2/O3 to OP4/P3 with less strain and enhanced Na + kinetics. These findings evidence that exploring novel multiphase cathodes is an effective approach to improve the electrochemical performances of cathode for sodium-ion batteries.
研究领域:
材料科学
·
电化学
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ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Xu Fu,Wen Yin,Dao Shi,Yifan Yang,Suisui He,Jun Hai,Zhenqing Hou,Zhongxiong Fan,Dekui Zhang
The synergistic nanotheranostics of reactive oxygen species (ROS) augment or phototherapy has been a promising method within synergistic oncotherapy. However, it is still hindered by sophisticated design and fabrication, lack of a multimodal synergistic effect, and hypoxia-associated poor photodynamic therapy (PDT) efficacy. Herein, a kind of porous shuttle-shape platinum (IV) methylene blue (Mb) coordination polymer nanotheranostics-loaded 10-hydroxycamptothecin (CPT) is fabricated to address the abovementioned limitations. Our nanoreactors possess spatiotemporally controlled O2 self-supply, self-sufficient singlet oxygen (1O2), and outstanding photothermal effect. Once they are taken up by tumor cells, nanoreactors as a cascade catalyst can efficiently catalyze degradation of the endogenous hydrogen peroxide (H2O2) into O2 to alleviate tumor hypoxia. The production of O2 can ensure enhanced PDT. Subsequently, under both stimuli of external red light irradiation and internal lysosomal acidity, nanoreactors can achieve the on-demand release of CPT to augment in situ mitochondrial ROS and highly efficient tumor ablation via phototherapy. Moreover, under the guidance of near-infrared (NIR) fluorescent imaging, our nanoreactors exhibit strongly synergistic potency for treatment of hypoxic tumors while reducing damages against normal tissues and organs. Collectively, shuttle-shape platinum-coordinated nanoreactors with augmented ROS capacity and enhanced phototherapy efficiency can be regarded as a novel tumor theranostic agent and further promote the research of synergistic oncotherapy.
研究领域:
纳米技术
·
癌症治疗
·
生物医学工程
·
光疗
·
药学
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高影响因子
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