WATER RESEARCH
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2023
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IF 12.8
Xixi Chen,Wanyi Fu,Zhichao Yang,Yulong Yang,Yanjun Li,Hui Huang,Xihui Zhang,Bingcai Pan
Hydrogen peroxide (H 2 O 2 ) is the most commonly used oxidant in advanced oxidation processes for emerging organic contaminant degradation. However, the activation of H 2 O 2 to generate reactive oxygen species is always accompanied by O 2 generation resulting in H 2 O 2 waste. Here, we prepare a Ti doped Mn 3 O 4 /Fe 3 O 4 ternary catalyst (Ti-Mn 3 O 4 /Fe 3 O 4 ) to create abundant oxygen vacancies (OVs), which yields electron delocalization impacts on enhancing the electrical conductivity, accelerating the activation of O 2 to produce H 2 O 2 . In Ti-Mn 3 O 4 /Fe 3 O 4 /H 2 O 2 system, OVs-mediated O 2 /O 2 •− /H 2 O 2 redox cycles trigger the activation of locally generated O 2 , boost the regeneration of O 2 •− and on site produce H 2 O 2 for replenishment. This leads to a 100% removal of tiamulin in 30 min at an unprecedented H 2 O 2 utilization efficiency of 96.0%, which is 24 folds higher than that with Fe 3 O 4 /H 2 O 2 . Importantly, further integration of Ti-Mn 3 O 4 /Fe 3 O 4 catalysts into membrane filtration achieved high rejections of tiamulin (> 83.9%) from real surface water during a continuous 12-h operation, demonstrating broad pH adaptability, excellent catalytic stability and leaching resistance. This work demonstrates a feasible strategy for developing OVs-rich catalysts for improving H 2 O 2 utilization efficiency via activation of locally generated oxygen during the Haber-Weiss reaction.
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ACS Applied Materials & Interfaces
·
2023
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IF 9.5
Wenqing Hou,Chen Chen,Diya Xie,Yiming Xu
Metal–organic frameworks (MOFs) as photocatalysts have received increasing attention. In this work, a dual metal-substituted UiO-66-NH2 (Ti/Ce-MOF) containing different Ti/Ce mole ratios (x = 0–2.46) has been prepared via post-synthetic exchange between Ce-UiO-66 and TiCl4, followed by amination. The solid had a high surface area (828–937 m2/g) and a large pore volume (0.451–0.507 m3/g). Under visible light, Ti/Ce-MOF showed x-dependent activity for H2O reduction and oxidation on a film electrode, respectively. However, such a change for H2 evolution in a Na2S/Na2SO3 aqueous solution was observed only after CdS loading. In combination with the photoluminescence and band parameters, we propose that the photoactivity of Ti/Ce-MOF for redox reaction is determined by its ability for electron transfer. Furthermore, there is an interfacial electron transfer from Ti/Ce-MOF to CdS and a hole transfer from CdS to Ti/Ce-MOF, respectively, significantly improving the efficiency of charge separation for redox reactions. This work offers a new insight that Ti substitution benefits the performance of Ce-based MOF.
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ACTA MATERIALIA
·
2023
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IF 9.4
Ruineng Ruan,Haibo Xiao,Wenjing Dong,Zhanghong Yu,Xunying Wang,Baoyuan Wang,Chen Xia,Hao Wang
Fast ionic transportation is in high demand for developing low-temperature solid oxide fuel cells (LT-SOFCs). Facing this challenge, a new H + /O 2− /Li + triple conductor is designed in this study from a lithium-metal oxide, spinel Li 4 Ti 5 O 12 (LTO). First-principle calculation based on density functional theory (DFT) reveals the proton transport barrier in LTO can be as low as 0.37 eV while the barrier for oxygen ion transportation is 0.94 eV. Using the designed LTO as the electrolyte and a typical cathode of lithium-ion battery, LiNi 0.8 Co 0.15 Al 0.05 O 2-δ , as the symmetrical electrodes, an all-lithium-metal-oxides-based LT-SOFC is constructed. High performance is achieved by the SOFC at 550–425 °C, i.e. 625 mW cm −2 at 550 °C, and a low activation energy of 0.60 eV is found with respect to the ionic conductivity of LTO at 550–475 °C. Further study confirms the dual O 2− /H + conduction of LTO via the application of proton and oxygen ion filters as well as the transference number test. Additionally, particular attentions are paid to the transport behavior of Li + in the cell via a charging process study and from XRD results. The possible contribution of triple conduction on fuel cell performance is discussed. This work demonstrates the great promise of triple H + /O 2− /Li + conducting lithium-metal oxides for LT-SOFC electrolyte development.
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JOURNAL OF ELECTRONIC MATERIALS
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2023
·Vol. 52
·期 10
·6613-6624
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IF 2.1
Gong Huixia,Wang Liqin,Wang Jianshe,Liu Qingchao
Lithium-oxygen (Li-O 2 ) batteries have become one of the most promising next-generation energy storage systems due to their high theoretical specific capacity. However, Li-O 2 batteries still face the problem of high charging voltage due to incomplete decomposition of discharge products. Here, a nitrogen-doped hollow spherical carbon composite containing Ni/Co nanoparticles was prepared by hydrothermal and pyrolysis strategies, and used as positive catalyst for Li-O 2 batteries to adjust the morphology of the discharge product. The porous hollow carbon sphere provides sufficient space for the storage of discharge products. Nitrogen-doped carbon nanospheres can change the local charge density, improve the electron transfer performance, and reduce the resistivity of carbon nanospheres. In addition, the abundant M-N x active groups enhance the affinity of the positive electrode to the reaction intermediates, thus regulating the morphology of the discharge product Li 2 O 2 . Benefiting from the above synergistic advantages, the electrochemical performance of the Li-O 2 battery including round-trip efficiency, discharge capacity, and cycling stability is greatly improved. Graphical Abstract
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
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IF 5.518
Linfeng Peng,Hang Yin,Lu Zou,Faquan Yu
As a promising energy storage technology, Li-CO 2 /O 2 batteries not only deliver ultrahigh discharge capacity but also capture and convert CO 2 into renewable energy. The exploration into the deposition and decomposition kinetics of discharge product (Li 2 CO 3 ) is urgent for the high thermodynamic stability. Herein, the influence of current density on the essential characteristics of Li 2 CO 3 has been explored. The results show that the Li 2 CO 3 with poor crystallinity and elliptical disk morphology can be obtained at medium current density, corresponding to the excellent electrochemical performance including ultrahigh capacity of 5800 mA h/g, lower discharge-charge gap of 1.15 V, and long-term cycle life of 80 cycles. In addition, the morphology and crystallinity of Li 2 CO 3 are tailored by the relative energy barriers for electron migration and O 2 - generation. At a medium current density (500 mA/g), the accelerated electron migration can realize the nucleation rate equivalent to growth one of Li 2 CO 3 . At this time, Li 2 CO 3 will uniformly deposit on the cathode surface, forming elliptical disk morphology with poor crystallinity. Obviously, this work provides new sights for promoting the development of Li-CO 2 /O 2 battery through rational design of catalysts to accelerate the deposition and decomposition processes of Li 2 CO 3 .
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CHEMOSPHERE
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2022
·
IF 8.943
Wanying Xie,Wei Song,Ji Li,Xiaolei Zhang,Wenyi Dong,Feiyun Sun
Modifying PVDF membrane by blending hydrophilic nano TiO 2 has been highly concerning, but its practical application is not well investigated. In this study, PVDF-TiO 2 membrane was employed in two modes to treat micro-polluted raw water for the first time, direct membrane filtration and pre-oxidation assists membrane filtration. At two filtration modes, the PVDF-TiO 2 membrane had comparable rejection capability to the unmodified PVDF membrane, as the removal of permanganate index (COD Mn ) was 0.26–0.72 mg/L, UV 254 was 0.0070–0.0618 cm −1 , turbidity was 1.60–4.49 NTU, and the total number of colonies was 360–23,780 CFU/mL. As for raw water treatment , using Fe 2+ /sodium dithionite (DTN)/O 2 system as the pre-oxidation process to assist the filtration of the PVDF-TiO 2 membrane was feasible. After optimization, the applicable conditions of the Fe 2+ /DTN/O 2 process were DTN dosage at 100 mg/L and a C Fe / C DTN of 1:4. As a result, the effluent qualities of the PVDF-TiO 2 membrane significantly improved. It was investigated that atrazine (ATZ), COD Mn , UV 254, and turbidity reduced, which was realized by the synergic effects of the pre-oxidation by free radicals and flocculation by iron. Pre-oxidation of the Fe 2+ /DTN/O 2 process could also enhance the permeability of the PVDF-TiO 2 membrane from 53.6 to 58.0 L/(m 2 ·h), nearly two times the PVDF membrane. Besides, the practical fouling of the PVDF-TiO 2 membrane was stably alleviated by the reduced R t , R re, and R ir , mainly due to constraining the internal pore fouling effectively.
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ACS Applied Energy Materials
·
2022
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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 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
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电池技术
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材料科学
·
电化学
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2018
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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
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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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