ACS Catalysis
·
2022
·
IF 13.7
Liu Lin,Youxuan Ni,Long Shang,Haoxiang Sun,Qiu Zhang,Wei Zhang,Zhenhua Yan,Qing Zhao,Jun Chen
Regulating the atomic arrangement and electron redistribution is beneficial for tuning catalytic oxygen reduction reaction (ORR) performance and deciphering the intrinsic mechanism. Herein, we modulate the charge density around Co centers by designing and synthesizing three Co coordination polymer catalysts, including Co-DABDT (DABDT = 2,5-diaminobenzene-1,4-dithiol, Co–N2S2), Co-BTT (BTT = 1,2,4,5-tetramercaptobenzene, Co–S4), and Co-BTA (BTA = 1,2,4,5-benzenetetramine, Co–N4), to explore the structure–activity relationship between the coordination environment and ORR performance. Because of the high electronegativity of S compared to N atoms, the charge density of Co increases in the order of Co-BTA → Co-DABDT → Co-BTT. Experimentally, Co-DABDT@CNTs with Co–N2S2 delivers a remarkable half-wave potential of 0.85 ± 0.002 V, outperforming Co–N4 and Co–S4 and even Pt/C (0.84 ± 0.003 V). Zinc–air batteries using Co-DABDT@CNTs as the air cathode catalyst also demonstrate excellent power density and stability. The systematic characterization and theoretical simulation reveal that the charge redistribution on Co and S sites of Co–N2S2 would both effectively optimize and stabilize the key intermediate (OOH*) with the assistance of hydrogen bonding interactions between intermediates and active S atoms (*OO–H···S). Interpreting the mechanism of ORR in the coordination sphere provides a feasible way to improve catalytic activity at an atomic level.
✓ 已验证
DOI
高影响因子
Small
·
2024
·
IF 13
Songzhu Xing,Xujiao Ma,Qingqing Gu,Nana Ma,Zhong Zhang,Guoying Han,Rui Huang,Xiao Feng,Bing Yang,Chunying Duan,Yiwei Liu
The construction of defective sites is one of the effective strategies to create high-activity Metal–Organic frameworks (MOFs) catalysts. However, traditional synthesis methods usually suffer from cumbersome synthesis steps and disordered defect structures. Herein, a cluster–cluster co-nucleation (CCCN) strategy is presented that involves the in situ introduction of size-matched functional polyoxometalates (H 6 P 2 W 18 O 62 , {P 2 W 18 }) to intervene the nucleation process of cluster-based MOFs (UiO-66), achieving one-step inducement of exposed defective sites without redundant post-processing. POM-induced UiO-66 ({P 2 W 18 }-0.1@UiO-66) exhibits a classical reo topology for well-defined cluster defects. Moreover, the defective sites and the interaction between POM and skeletal cluster nodes are directly observed by Integrated Differential Phase Contrast in Scanning Transmission Electron Microscopy (iDPC-STEM). Owing to the molecular-level proximity between defective sites and POM in the same nano-reaction space, {P 2 W 18 }-0.1@UiO-66 exhibits efficient tandem catalysis in the preparation of γ-valerolactone (γ-GVL) from laevulinic acid (LA) by the combination of Lewis and Brønsted acids with 11 times higher performance than defective UiO-66 formed by conventional coordination modulation strategy. The CCCN strategy is applicable to different POM and has the potential to be extended to other cluster-based MOFs, which will pave a new way for the construction of functional MOFs with multi-centered synergistic catalysis.
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF ELECTRONIC MATERIALS
·
2016
·Vol. 45
·期 6
·2974-2980
·
IF 1.491
Zheng Yuhui,Hu Jing,Deng Surong,Gao Jinwei,Wang Qianming
High-purity LuVO 4 : Ln 3+ /Bi 3+ (Ln = Eu, Sm, Dy) phosphors with tetragonal zircon structures were successfully synthesized. The reactions have been carried out by multiple irradiations with very high efficiency. Transmission electron microscope images showed that the phosphors had rod-like structures with average lengths of about 200 nm. The host absorption edge of LuVO 4 : Ln 3+ /Bi 3+ (Ln = Eu, Sm) shifted to the longer wavelength side. Furthermore, the red emission of Eu 3+ ion and the orange emission of Sm 3+ ion are remarkably enhanced by encapsulating Bi 3+ in LuVO 4 system, whereas in the case of LuVO 4 : Dy 3+ /Bi 3+ , the host absorption and the yellow emission from dysprosium have been suppressed in the presence of Bi 3+ . These novel findings will facilitate their use in the display field.
✓ 已验证
DOI
高影响因子
Frontiers in Energy Research
·
2022
·
IF 3.858
Ye Xiaodong,Jiang Yangyang,Chen Xi,Guo Benshuai,Mao Songbai,Guo Yafei,Zhao Chuanwen
Electrochemical CO2 reduction to CO using copper-based catalysts has been recognized a promising approach to realizing anthropologic carbon cycle. However, copper-based catalysts face the challenges of low reduction activity and poor selectivity in CO2 reduction reaction. Tuning particle size and oxygen vacancy represents an efficient strategy for boosting their activity and selectivity. Herein, we reported the preparation of nanostructured CuO catalysts for selective electrochemical CO2 reduction to CO. Several templates were employed in the template-assisted hydrothermal process to regulate the particle size and oxygen vacancy. Structure-property-activity relationships of the CuO nanostructures depend on the template effect. CuO-PVP and CuO-SDS synthesized using polyvinylpyrrolidone (PVP) and sodium dodecyl sulfate (SDS) as templates exhibited smaller particles sizes and higher concentrations of oxygen vacancy defects. Under the applied potential of −0.93 V vs. RHE, the desired CuO-PVP and CuO-SDS catalysts exhibited good CO2 reduction activity with high electrochemical surface area normalized partial current density of 2.21 and 1.37 mA/cm2 for CO production and outstanding CO selectivity with high faradaic efficiencies of 48.2 and 50.5%. Density functional theory (DFT) calculations indicated that oxygen vacancies in the CuO nanostructures not only promoted CO2 adsorption and activation but facilitated CO desorption from the catalyst surface, and therefore boosted the activity and CO selectivity in CO2 reduction. The results have deepened the understanding of the structure-property-activity relationships of CuO catalysts, and these will provide guidance for designing highly efficient and robust catalysts for electrochemical CO2 reduction to CO.
✓ 已验证
DOI
高影响因子
RSC Advances
·
2020
·Vol. 10
·期 4
·1956-1965
·
IF 3.119
Weiqi Xie,Shiwen Huang,Donglin Tang,Shumei Liu,Jianqing Zhao
A furfural-based DOPO-containing flame retardant, 6,6′-(((methylenebis(4,1-phenylene))bis(azanediyl))bis(furan-2-ylmethylene))bis(dibenzo[c,e][1,2]oxaphosphinine 6-oxide) (MBF-DOPO), was synthesized and utilized as a co-curing agent of 4,4′-diaminodiphenyl methane (DDM) for fire-safe epoxy thermosets. For the cured epoxy resin containing 4.0% MBF-DOPO, the limiting oxygen index (LOI) reached 32.9% (with the V-0 rating in UL-94 test), and the peak heat release rate and total smoke production values were respectively decreased by 29.3% and 33.6%, compared to pure epoxy resin. Scanning electron microscopy (SEM) and Fourier transform infrared spectroscopy (FTIR) results confirmed that the furfural-based flame retardant MBF-DOPO promoted the charring formation of the epoxy matrix, which effectively isolated the gas and heat transfer during combustion and thus enhanced the fire-safety performance of the epoxy thermosets. This work provides an effective route for synthesizing a furfural-based flame retardant, which possesses great potential for application in fire-safe epoxy thermosets.
✓ 已验证
DOI
高影响因子
Polymer Chemistry
·
2021
·Vol. 12
·期 31
·4524-4531
·
IF 5.582
Xiaoqing Ai,Jiansen Pan,Qingyi Xie,Chunfeng Ma,Guangzhao Zhang
Hyperbranched polymers with high solubility, low viscosity, low crystallinity and dense functional groups are promising to be used in adhesives and coatings. In this study, we have developed a cleavable hyperbranched poly(ester-co-vinyl) with diethylene glycol units and unreacted pendant vinyl groups via radical ring-opening copolymerization of 2-methylene-1,3-dioxepane (MDO), vinyl acetate (VAc) and diethylene glycol divinyl ether. Such a hyperbranched polymer with vinyl groups can form a crosslinked network by UV curing. The cleavable ester bonds are randomly distributed in the main chain, so they can degrade into small fragments with molar masses of 400–600 g mol−1. The degradation rate can be well regulated with MDO content. The protein resistance, antibacterial adhesion and anti-diatom activity of the hyperbranched polymer were examined. The polymer with diethylene glycol units exhibits remarkable antifouling abilities and can effectively inhibit the adhesion of protein, marine bacteria (Pseudomonas sp.) and diatoms (Navicula incerta). The hyperbranched polymer coating can find application in marine antifouling.
✓ 已验证
DOI
高影响因子
RSC Advances
·
2020
·Vol. 10
·期 11
·6287-6296
·
IF 3.119
Zhikun Liu,Yanhong Yin,Daijun Yang,Cunman Zhang,Pingwen Ming,Bing Li,Shuting Yang
A simple and efficient method was used to prepare highly active and durable carbon-supported ultrathin Pt–Co nanowires (NWs) as oxygen reduction reaction (ORR) catalysts for the cathode in a proton exchange membrane fuel cell (PEMFC). Chromium hexacarbonyl plays a significant role in making Pt and Co form an alloyed NW, which acts as both a reducing agent and a structure directing agent. The nanocrystal exhibits a uniform nanowire morphology with a diameter of 2 nm and a length of 30 nm. In half cell tests, the Pt–Co NWs/C catalyst has a mass activity of 291.4 mA mgPt−1, which is significantly better than commercial Pt/C catalysts with 85.5 mA mgPt−1. And after the accelerated durability test (ADT), Pt–Co NWs/C shows an electrochemically active surface area (ECSA) loss of 19.1% while the loss in the commercial catalyst is 41.8%. Also, the membrane electrode assembly (MEA) was prepared using Pt–Co NWs/C as the cathode catalyst, resulting in a maximum power density of 952 mW cm−2, which is higher than that of Pt/C. These results indicate that the one-dimensional structure of the catalyst prepared herein is favorable to improve the activity and durability, and the application of the catalyst in the MEA is also realized.
✓ 已验证
DOI
高影响因子
EUROPEAN JOURNAL OF SOIL BIOLOGY
·
2024
·
IF 3.7
Zongyang Liu,Shenghao Ai,Meihua Sheng,Jingyao Xiao,Peng Wang,Yingwei Ai,Xiaoyan Ai
Soil organic phosphorus (OP) mineralization plays a vital role in the ecological restoration of roadside slopes. However, the changes in the functional bacterial ( phoD -harboring) community involved in OP mineralization in soil aggregates during slope restoration are still unknown. In this study, a space-for-time substitution was conducted to compare the differences in the phoD -harboring bacterial community structure and assembly in soil aggregates of four particle sizes (<0.053, 0.25–2, 0.053–0.25, and >2 mm) at different slope restoration ages (7, 11, and 14 years). The results showed no significant differences in the phoD -harboring community diversity and structure among soil aggregates in the same restoration year. Community structure dissimilarity increased with restoration time. Species replacement dominated slope soils restored for 7, 11, and 14 years, accounting for 78.40 %, 79.68 %, and 68.96 % of the total β-diversity, respectively. Community assembly processes shifted from coexisting deterministic (68 %) and stochastic (32 %) processes in the 7-year restoration slope soil to dominantly deterministic (98 % and 91 %) processes in the 11- and 14-year restoration slope soils, respectively. Dominant phoD -harboring bacteria tended to shift from r-to K-strategies as slope restoration progressed, and the C:P ratio significantly correlated with both community structure and assembly. The increasing C:P ratio over restoration time stimulated phoD -harboring bacteria to secrete alkaline phosphatase to improve P availability, enhancing the complexity and stability of the network. This study elucidates the changing patterns of phoD -harboring bacteria in soil aggregates and provides a theoretical basis for the management of soil P during roadside restoration.
✓ 已验证
DOI
高影响因子
MODERN PHYSICS LETTERS B
·
2024
·
IF 1.8
Li Liu,Qifu Bao,Tiangui Zhao,Kun Liu,Detai Shi,Siyu Li,Wei Zhu,Xiaolong Li,Jianer Zhou
A series of Zn 1 − x Fe x O ( x = 0 , 0.015, 0.045, 0.075) nanoparticles were synthesized using the solution co-precipitation method, and their structural and property characteristics were investigated. X-ray diffraction (XRD) analysis revealed that all Zn 1 − x Fe x O samples exhibited a hexagonal wurtzite crystal structure with the P63mc space group. The introduction of Fe doping led to a slight lattice distortion in the samples. The morphology of the nanoparticles, including polydispersion and agglomeration, as well as the presence of the second phase ZnFe 2 O 4 , was examined by scanning electron microscope (SEM) and transmission electron microscope (TEM). UV–Vis diffuse reflectance spectroscopy demonstrated that the band gap of Zn 1 − x Fe x O lies between 3.152 and 3.163 eV. With the increase in Fe ion doping, the band gap shows a slight decreasing trend. Mössbauer spectroscopy revealed that iron ions in the nanoparticles existed in a trivalent state and exhibited two different configurations: One involved iron replacing zinc without creating a vacancy, while the other involved iron substituting zinc with a vacancy. The ferromagnetic nature of the Fe-doped samples can be attributed to the exchange interaction between two Fe 3 + ions mediated by the F-center mechanism.
✓ 已验证
DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
Yao Huang,Shufeng Zhao,Hui Liu,Rong Chen,Lei Zhao,Shan Liu
Abiotic Fe (II) oxidation widely occurs in the natural subsurface environment and engineered dynamic processes, which possibly impacts the growth of indigenous microbes. As previously discovered, the oxidation of aqueous Fe 2+ at neutral pH effectively inactivates iron-reducing bacteria Shewanella oneidensis strain MR-1 (MR-1). Herein, the impacts of co-existing iron mineral on the oxidation of aqueous Fe 2+ and the subsequent disinfection activity on MR-1 were investigated with siderite selected as a representative iron mineral in the subsurface environment. The oxidation rate of aqueous Fe 2+ and the amount of generated OH radical increased as the content of siderite increased, while the MR-1 inactivation was alleviated. An initial concentration of 2.0 × 10 6 CFU/mL MR-1 was inactivated by about 2.7 orders of magnitude during oxidation of 0.2 mM FeSO 4 alone for 30 min, which was reduced to only about 0.6 orders of magnitude in the presence of 4.3 mM co-existing siderite. ROS scavenging results confirmed that the OH radical generated in the bulk solution was not the leading role for the inactivation of MR-1. Morphological changes of the cells observed by SEM demonstrated that the disruption of the cell membrane was alleviated by siderite, which was further supported by the XRD and FTIR spectra. The underlying mechanism was proposed to be the reduced contact time of Fe 2+ and MR-1 cells due to the accelerated oxidation. This work provides new insights into the disinfection behavior of heterogeneous Fe (II) oxidation on iron cycling bacterial in the natural environment.
✓ 已验证
DOI
高影响因子
Nanomaterials
·
2022
·Vol. 12
·期 15
·2595
·
IF 5.719
Xian Zhou,Xia Chen,Wei Han,Yi Han,Mengxin Guo,Ziling Peng,Zeyu Fan,Yan Shi,Sha Wan
The sludge-derived biochar is considered an effective emerging contaminants adsorbent for wastewater treatment. In this paper, red mud and steel slag (RMSS) was used for improving sludge dewaterability and enhancing the sludge-derived biochar adsorption capacity. X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), and a scanning electron microscope (SEM) were employed to comprehensively characterize the mineral composition, functional group, and morphology of the adsorbent. RMSS was able to improve the sludge dewatering performance by providing a skeleton structure to promote drainage and Fe(III) to decrease the Zeta potential. The dosage of 20 mg/g RMSS was able to reduce the specific resistance to filtration (SRF) and the Zeta potential of sludge from 1.57 × 1013m/kg and −19.56 mV to 0.79 × 1013m/kg and −9.10 mV, respectively. The co-pyrolysis of RMSS and sludge (2:8) induced the formation of biochar containing FeAl2O4(PS80). The PS80 exhibited a large surface area (46.40 m2/g) and high tetracycline (TC) removal capacity (98.87 mg/g) when combined with H2O2(PS80-H2O2). The adsorption process of TC onto PS80 and PS80-H2O2was well described by the pseudo-first-order and pseudo-second-order kinetic model, indicating physisorption and chemisorption behavior. The results indicated that co-pyrolysis of RMSS sludge PS80-H2O2could enhance the biochar adsorption capacity of TC, attributable to the degradation by ·OH generated by the heterogeneous Fenton reaction of FeAl2O4and H2O2, the release of adsorbed sites, and the improvement of the biochar pore structure. This study proposed a novel method for the use of RMSS to dewater sludge as well as to induce the formation of FeAl2O4in biochar with effective TC removal by providing a Fe and Al source, achieving a waste-to-resource strategy for the integrated management of industrial solid waste and sewage sludge.
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Aziz-Ur-Rahim Bacha,Iqra Nabi,Hanyun Cheng,Kejian Li,Saira Ajmal,Tao Wang,Liwu Zhang
Bisphenol A (BPA) is known as an endocrine-disrupting chemical, generally present in the environment. It has a harmful effect on aquatic lives and human health, therefore it is needful to exploit highly efficient innovative treatment methods for its removal. Herein, we report a Co-BiVO 4 photoanode to activate peroxymonosulfate (PMS) for the complete removal of BPA via a photoelectrochemical (PEC) process. The Co-BiVO 4 could degrade 99.16% of BPA in the presence of 2 mM PMS within 60 min, whereas the degradation rate constant is 0.08034 min −1 , which was 20.86 times higher than the electrocatalytic (EC) and 5.35 times higher than the photocatalytic (PC) process. Notably, Co-BiVO 4 showed significant activity toward PMS activation and BPA degradation as compared to other synthesized photocatalysts. Their photoelectrocatalytic performance followed the sequence Co-BiVO 4 > Fe-BiVO 4 > Ni-BiVO 4 > pure-BiVO 4 > without catalysts. Several influencing factors on the decomposition process, such as the effect of PMS concentration, applied potential, illumination time, initial pH, BPA concentration, Co loading, and co-existing anions were studied in detail. Radical scavenging experiment and transient absorption result showed that sulfate radicals (SO 4 •─ ) were the dominant reactive species. Moreover, a significant synergistic effect was noticed in Co-BiVO 4 /PEC/PMS system for BPA degradation. Degradation mechanism and reaction intermediates were studied by in-situ diffuse reflectance infrared Fourier-transform spectroscopy (DRIFTS) and liquid chromatography-mass spectroscopy (LC-MS) presenting the enhanced bond cleavage in PEC activated PMS system. The BPA showed 92.47% and 87.27% removal in tap and river water samples after 60 min of reaction using Co-BiVO 4 /PMS PEC system. Our finding proposed an efficient method for wastewater treatment in an eco-friendly way.
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）