ACTA MATERIALIA
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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 MATERIALS SCIENCE & TECHNOLOGY
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2023
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IF 10.9
Yunbo Feng,Qian Wang,Shudong Sun,Weifeng Zhao,Changsheng Zhao
Artificial lung membranes as the core module of the extracorporeal membrane oxygenation technology (ECMO) execute the function of extracorporeal blood-gas barrier accomplishing CO 2 /O 2 exchange with blood. However, the unsatisfactory hemocompatibility and difficulty in functionalization are the prominent challenges faced by current artificial lung membrane materials. In this study, polyethersulfone (PES) composite membranes with self-anticoagulant property and high gas exchange efficient are fabricated by blending PES matrix with poly(vinylamine) (PVAm) modified carboxylic carbon nanotubes (mCNTs) and citrate-based poly(octamethylene-citrate) (POC) pre-polymers. The mCNTs construct specific gas transfer channels within the composite membranes to enhance the gas permeability, while the POC pre-polymers provide anticoagulant property based on the chelation to blood Ca 2+ and the inactivation effect to intrinsic coagulation factors. Importantly, directed by the actual ECMO gas exchange mode, we design a gas-liquid convectional circulation device that could evaluate gas exchange efficiency for the composite membranes under mimetic ECMO state. Therefore, this strategy not only proposes a new design method of advanced artificial lung membranes to solve the practical challenges in the current ECMO technology, but also establishes a scientific testing method to evaluate the gas exchange performance for new-type artificial lung membrane materials in the future.
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JOURNAL OF THE EUROPEAN CERAMIC SOCIETY
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2023
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IF 5.7
Yulan Yu,Guanghui Feng,Yujun Jia,Hejun Li
In this work, AlN whisker-reinforced (Zr, Hf)O 2 coating was prepared on SiC coated carbon/carbon composites by sol-gel and plasma spraying methods. Its cyclic ablation resistance was evaluated using an oxyacetylene torch with a heat flux of 2.38 MW/m 2 . After ablation, the coating showed apparently decreased crack sizes and quantity as compared with the one without AlN whisker addition, pointing out its better crack tolerance. Moreover, the coating had a thinner oxidized region based on the linear ablation rate (−0.042 µm/s), greatly lower than that of pure oxide coating (−0.922 µm/s). After detailed observation and characterization, probable protection mechanism was proposed.
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Journal of Environmental Sciences
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2023
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IF 6.9
Yi Yuan,Wen-Long Wang,Zhi-Wei Wang,Jin Wang,Qian-Yuan Wu
Carbon nitride has been extensively used as a visible-light photocatalyst, but it has the disadvantages of a low specific surface area, rapid electron–hole recombination, and relatively low light absorbance. In this study, single-atom Ag was successfully anchored on ultrathin carbon nitride (UTCN) via thermal polymerization, the catalyst obtained is called AgUTCN. The Ag hardly changed the carbon nitride's layered and porous physical structure. AgUTCN exhibited efficient visible-light photocatalytic performances in the degradation of various recalcitrant pollutants, eliminations of 85% were achieved by visible-light irradiation for 1 hr. Doping with Ag improved the photocatalytic performance of UTCN by narrowing the forbidden band gap from 2.49 to 2.36 eV and suppressing electron–hole pair recombination. In addition, Ag doping facilitated O 2 adsorption on UTCN by decreasing the adsorption energy from −0.2 to −2.22 eV and favored the formation of O 2 ·− . Electron spin resonance and radical-quenching experiments showed that O 2 ·− was the major reactive species in the degradation of Acetaminophen (paracetamol, APAP).
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PubMed
高影响因子
ACS Applied Materials & Interfaces
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2023
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IF 9.5
Qiuli Wang,Jiahao Meng,Lingling Huang,Feng Wu,Xue Yi,Guanghao Su,Ying Li,Zhenqing Hou,Zhongxiong Fan
How to efficiently synthesize toxic chemo-drugs in the hypoxia tumor microenvironment still faces a huge challenge. Herein, we have tailored engineered vehicle-free nanoreactors by coordination-driven co-assembly of photosensitizer indocyanine green (ICG), transition metal platinum (Pt), and nontoxic 1,5-dihydroxynaphthalene (DHN) to self-amplify O2 and cascade chemo-drug synthesis in tumor cells for self-reinforcing hypoxic oncotherapy. Once vehicle-free nanoreactors are internalized into tumor cells, they show a serious instability that results in rapid disassembly and on-demand drug release under the stimuli of acidic lysosome and laser radiation. Notably, the released Pt can efficiently decompose the endogenous hydrogen peroxide (H2O2) into O2 to alleviate tumor hypoxia, which is conducive to enhancing the photodynamic therapy (PDT) efficiency of the released ICG. Complementarily, a large amount of the 1O2 generated by PDT can efficiently oxidize the released nontoxic DHN into the highly toxic chemo-drug juglone. Therefore, such vehicle-free nanoreactors can achieve intracellular on-demand cascade chemo-drug synthesis and self-reinforce photo-chemotherapeutic efficacy on the hypoxic tumor. On the whole, such a simple, flexible, efficient, and nontoxic therapeutic strategy will broaden the study of on-demand chemo-drug synthesis and hypoxic oncotherapy.
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ACS Applied Materials & Interfaces
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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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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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CHEMOSPHERE
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2022
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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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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Yuancheng Qin,Zhenhua Jiang,Yue Guo,Muhammad Asim Mushtaq,Zhen Shen,Wanjun Du,Cailing Ni,Geng Luo,Yu Ji,Zhiqi Zhang,Yonggui Deng,Arshad Hussain,Lasharl Najeeb Ur Rehman,Xingke Cai,Panagiotis Tsiakaras,Jie Zhao
Porous organic polymers (POPs) have emerged as functional materials in photocatalytic degradation of tetracycline (TC) antibiotics but still did not get enough attention on the degradation mechanism and “structure-performance” relationship. It is of great scientific concern to explore the photo-degradation capability of POPs for TC antibiotics under visible light and to reveal their “structure-performance” relationship at the molecular level. Herein, we have constructed a novel benzotriazole-based POP by polymerizing benzotriazole-based structure with melamine. The photo-degradation test results indicate that the POP with benzotriazole-based structure presents an excellent photocatalytic performance with a high TC removal efficiency of 92.12 % and good recyclability. The corresponding pseudo-first-order reaction kinetic constant of benzotriazole-based POP is 6.8 times that of benzene-based one. Such excellent performance of benzotriazole-based POP can be attributed to the physical/chemical property contributions of benzotriazole-based structure to POP, e.g. , the narrow energy bandwidth (2.48 eV) for producing more photo-generated electrons/holes, the small charge transfer resistance for circumventing recombination of photo-generated electrons/holes, and the large number of O 2 − radicals converted from high-activated O 2 that produced by the interactions between photocatalyst and O 2 under visible light irradiation. This strategy of introducing the benzotriazole-based structure into POP opens new avenues to develop next-generation advanced photocatalysts for removing TC antibiotics from wastewater.
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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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ENVIRONMENTAL RESEARCH
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2022
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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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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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