Nanoscale
·
2022
·Vol. 14
·期 45
·17044-17052
·
IF 8.307
Lili Gao,Peng Wang,Huan Chai,Shuwen Li,Jun Jin,Jiantai Ma
Regarding the indirect hole transfer route in hematite-based photoelectrodes, the widely accepted viewpoint is that the FeIVO states act as a hole transfer medium, while other types of surface states act as recombination centers. Alternatively, it has rarely been reported that the recombining surface states may contribute to the charge transport in modified photoelectrodes. In this study, we employed CoCr layered double hydroxide (LDH)/Fe2O3 and CoCr LDH/Zr:Fe2O3 as research models to investigate the distinct charge transfer pathways in composite photoanodes. Different from the adverse role of surface states at ∼0.7 V versus the reversible hydrogen electrode (r-SS) in the bare hematite photoelectrodes (Fe2O3 or Zr:Fe2O3), the r-SS in the composite photoanodes (CoCr LDH/Fe2O3 or CoCr LDH/Zr:Fe2O3) served as a hole transfer station to induce high-valent Co cations, and the position of r-SS determined the onset potential of the composite photoelectrodes. Moreover, the FeIVO states still acted as active intermediates to transport numerous holes to the cocatalyst, which enhanced the charge utilization efficiency at 1.23 V versus the reversible hydrogen electrode (RHE) to a large extent. Besides, a noteworthy fact is that Zr doping increased the number of active FeIVO states, which significantly contributed to the enhancement in current density. However, it led to a delayed onset potential because of the positively shifted surface states (r-SS and FeIVO). Evidently, the different surface state distributions between Fe2O3 and Zr:Fe2O3 gave rise to anisotropic charge transfer and recombination behavior in the composite photoanodes. This study gives extensive insight into the hole transfer route in composite photoanodes and reveals the surface state-tuning effects of dopants and cocatalysts, which are significant for a deep understanding of the surface states and optimal design of composite photoanodes via surface state modulation.
研究领域:
材料科学
·
光电化学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Jiesong Tan,Yiqing Zeng,Jiahao Chen,Yutang Kang,Jiangxiao Qiao,Feng Zhang,Feng Han,Zhaoxiang Zhong,Weihong Xing
Oily particulate matter (PM) filtration faces the problems of high pressure drop and difficult regeneration. Herein, vertical arrays of MnO 2 nanosheets was assembled on Zr doped TiO 2 (Zr-TiO 2 ) nanofibers to construct a core–shell structure MnO 2 @Zr-TiO 2 (CSMT-x) catalytic membranes for highly efficient oily PM filtration and decomposition. The confining effect of the ultrathin MnO 2 nanosheets enhances PM capture efficiency, and the increase of effective contact area between MnO 2 and oily PM accelerate the decomposition of oily PM. The optimized CSMT-3 catalytic membrane exhibited high gas permeability and redox capacity, outperforming the Zr-TiO 2 (Bare T) membrane with over 99.97 % PM filtration efficiency and a low pressure drop at the temperatures of 25–425 °C. The catalytic decomposition of PM prevented the accumulation of particles on the membrane surface, which inhibited the formation of cake layer. Therefore, the CSMT-3 membrane exhibited a slight increase in pressure drop (less than 120 Pa) even after 120 h long-term filtration. This work may contribute to the development of advanced multifunctional membranes for purification of oily PM.
研究领域:
材料科学
·
环境工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2022
·Vol. 33
·期 14
·11165-11173
·
IF 2.779
Gan Liqiang,Yang Fei,Liu Jingsong,Cao Lijia,Huang Xu,Yuan Honglan,Xian Cong,Zhang Wanli
Zr substituted Bi 0.5 Y 1.5− x Ca 1+ x Zr x V 0.5 Fe 4.5− x O 12 ( x = 0.00, 0.25, 0.50, 0.75, 1.00) samples were prepared via solid-state reaction method. The structure, morphology, electromagnetic properties of Zr-doped Bi 0.5 Y 1.5− x Ca 1+ x Zr x V 0.5 Fe 4.5− x O 12 were investigated by SEM, XRD, FT-IR, Raman, VSM, impedance analyzer, and vector network analyzer. The results showed that the Zr 4+ and Ca 2+ ions successfully entered the octahedral a-sites and dodecahedral c-sites, respectively. The saturation magnetization increased with the increase of doping concentration in low concentration range. However, the excessive dopant of diamagnetic Zr 4+ ions resulted in a decrease in the saturation magnetization, indicating that the crystal lattice appeared short-range antiferromagnetic order at the d-sites, and the samples changed from ferromagnetism to paramagnetism. Among them, Bi 0.5 Y 1.25 Ca 1.25 Zr 0.25 V 0.5 Fe 4.25 O 12 has the optimum comprehensive properties, M s = 17.254 emu/g, H c = 4.043 Oe, M r = 0.268 emu/g, Δ H = 81 Oe, ε r = 18.68 @ 1 MHz, and tan δ ε = 0.002. The as-prepared material has potential application in communication devices such as circulators and isolators.
研究领域:
材料科学
·
物理学
✓ 已验证
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Yawen Wu,Xueying Hou,Rui Guo
The presence of tetrachlorobisphenol A(TCBPA) in the environment is continually increasing, which has potential negative effects on human health. Therefore, it is important to develop new materials that can degrade these compounds using various modification techniques. Recently, the photocatalytic degradation of organic pollutants using peroxides has been widely used as the focus of several research studies. This study synthesized Zr-doped NiFe 2 O 4 (Zr-NiFe 2 O 4 ) metal complex materials using a co-precipitation method and applied them to catalyze the degradation of a typical halogenated bisphenol A pollutant using different phase-catalyzed peroxydisulfate (PS) compounds. The results showed that Zr-NiFe 2 O 4 significantly enhances the nitrogen-active adaptive catalytic action between the reactive species and (NH 4 ) 2 S 2 O 8 , exhibiting an excellent catalytic performance (99 %). The degradation rate could reach 90 % after 30 mins with the low concentration of TCBPA (20 mg•L –1 ). Furthermore, the degradation of TCBPA in the Zr-NiFe 2 O 4 /LED/(NH 4 ) 2 S 2 O 8 system occurred over a wide pH range of 3–11. The results of leaching metals were detected that the concentrations of the leached zirconium, nickel and iron ions declined to 0.018 mg•L −1 . In addition, the tri-metal synergistic effect of Zr-NiFe 2 O 4 not only significantly improved the TCBPA removal efficiency, but also enhanced the long-term stability of the composite material. Mechanistic studies revealed that ·OH and SO 4 ·– were involved in the TCBPA degradation process with ·OH being the primary active species, and the possible degradation pathways were deduced using mass spectrometry. The on-line infrared test experiments showed the disappearance of the hydroxyl and double bond within approximately 120 seconds. Moreover, the magnetic properties of Zr-NiFe 2 O 4 met the water recovery requirements, effectively reducing secondary pollution, and aligned with the practical needs for water treatment, providing data for the construction of efficient magnetic catalysts.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Chao Zhang,Yongsheng Gao,Haipeng Wang,Lulu Jiang,Delu Zhang,Shujun Ming,Guangying Fu,Chao Wang,Zhiguo Lv
The dry reforming of methane (DRM) could convert CH 4 and CO 2 into syngas, offering potential for greenhouse gas mitigation. However, DRM catalyst sintering and carbon deposition remain major obstacles. In this study, a highly dispersed PtNi alloy@Zr-doped 3D hollow flower-like MgAl 2 O 4 (AMO) spheres was prepared through a hydrophobic driving strategy. During a 50-hour test at 550 °C, the catalyst exhibited no significant decline in CH 4 and CO 2 conversion rates, demonstrating its excellent anti-sintering and anti-coking performance. The unique anti-coking performance can be attributed to Zr-induced oxygen vacancies, which enhance oxygen mobility and reduce carbon deposition. Besides, doped Zr increases basic active sites, enhancing CO 2 adsorption and activation, thus accelerating carbon species conversion. At 700 °C, the unique synergy between highly dispersed Pt and Ni enabled CH 4 and CO 2 conversion rates to reach 67.5 % and 73.8 %, respectively. The incorporation of Pt or Zr extends the Ni–Ni bond and partially coordinates with Ni, enhancing the stability of the Ni lattice. The reaction of CH 4 and CO 2 follows the Langmuir-Hinshelwood (L-H) mechanism, where both reactant molecules are adsorbed and activated on the metallic sites. Moreover, the effective energy barrier for the CH oxidation pathway is lower by 0.16 eV than that for the C oxidation pathway, which helps suppress the formation of carbon deposits.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Omega
·
2020
·
IF 2.87
Fengqing Xiong,Danni Chen,Chenglong Ma,Limei Cao,Ji Yang
Electrochemical oxidation has been considered as an efficient method to degrade pharmaceuticals and personal care products. Maintaining low power consumption while increasing the number of oxidation intermediates is deserving of exploring. Herein, Ti/SnO2–Sb/Zr0.3Ir0.7O2 was prepared by Zr doped into IrO2 and used for Sulfamethoxazole (SMX) degradation. The addition of Zr significantly increased the electrochemically active area and facilitated the catalyst to degrade SMX dramatically at a lower overpotential. The extremely outstanding lifetime of catalysts can reach 800 h during the accelerated life test, which showed excellent stability and developmental prospects. The overpotential at 10 mA·cm–2 is about 329 mV, indicating that this electrode has a high oxygen evolution reaction activity. Furthermore, the electrical efficiency per log order for the electrode is only 8.50 kW h m–3 at 4 V. Our research provides new anode electrochemical catalysts for the degradation of organic pollutants.
研究领域:
环境科学
·
材料科学
·
电化学工程
✓ 已验证
DOI
高影响因子
iScience
·
2024
·
IF 4.6
Jielin Huang,Jie Wang,Haonan Duan,Li Dong,Songsong Chen,Junping Zhang,Xiangping Zhang
Acidic and basic sites of catalysts are essential for CO 2 capture and activation. In this work, Zr, N-ZnO/ZnAl-LDH-IL composites in ionic liquid and methanol systems were fabricated, and applied to catalyze the synthesis of ethylene carbonate (EC) from ethylene glycol (EG) and CO 2 with about 4.76 mmol EC g Cat. −1 h −1 . The composites showed more strong basic sites due to the effective induction of reactive groups on the catalyst surface by Zr doping, resulting in an increase of pyridinic-N groups from 5.48% to 22.25%. More C atoms adjacent to pyridinic-N as strong basic sites was conducive to the activation of CO 2 and EG. In addition, the possible catalytic pathway and mechanism of the composites for synthesizing EC as well as the doping of La, Fe, Ce, and Cu were also investigated, which provides an effective strategy for regulating the acid-base centers on the catalyst surface through ionic liquids and methanol solvents.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
NANO
·
2016
·
IF 0.951
Jimin Du,Huiming Wang,Huijuan Chen,Menghe Yang,Xiaoling Lu,Hui Guo,Zhanmin Zhang,Tianwei Shang,Shujue Xu,Wenqi Li,Pianpian Wang,Imran Shakir
Black Porous Zr-doped TiO 2 monoliths were successfully synthesized by a combined route including sol–gel method with polystyrene spheres as template followed by calcination at high temperature in the presence of oxygen. As-synthesized samples were then treated in hydrogen atmosphere at 500 ∘ C for 6 h to obtain black Porous Zr-doped TiO 2 monoliths. This as-synthesized black porous Zr-doped TiO 2 composite showed relatively narrow bandgap compared to the pure anatase phase of TiO 2 , which may have its origin from the contributions from the Zr impurity and oxygen vacancies. The photocatalytic activity of the black porous Zr-doped TiO 2 monolith was examined by carrying out the dye degradation on Rhodamine B under visible irradiation. Our experimental results indicate that black porous 0.9% Zr-doped TiO 2 sample exhibits high photocatalytic activity with the photodecomposition of 95.25% under visible irradiation for 120 min.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
Nano Energy
·
2025
·
IF 17.1
Zhao Sun,Huicai Wang,Xingxu Wang,Riguang Zhang,Zhiqiang Sun
Sorption-enhanced steam reforming of methanol (SE-SRM) offers a promising route for high-quality hydrogen production with in situ CO 2 capture; however, achieving an optimal balance between catalytic activity and CO 2 uptake capability, while ensuring catalyst stability, remains a significant challenge. In this study, a series of Zr-doped (0 wt%, 5 wt%, 15 wt%, 25 wt%) Cu-MgO catalytic sorbents are synthesized for SE-SRM. At 180℃, the hydrogen concentration and yield reach nearly 100 % and 10.35 μmol·g −1 ·s −1 . Moreover, the catalytic sorbent basically retains its catalytic activity and CO 2 uptake capacity after 30 cycles with merely slight deactivation. Results demonstrate that the doped Zr, presents as tetragonal ZrO 2 , enhances metal-support interactions with the formation of a Cu-O-Zr interfacial structure, promoting Cu nanocluster dispersion and altering the Cu + /Cu 0 distributions. Zr doping also enables the modulation of the medium-strong basic sites. Moreover, the AFM and TEM confirmed the formation of high-roughness MgO surface on the substrate, thereby facilitating CO 2 diffusion and adsorption. DFT calculation results further confirm the advantages of Zr-doped Cu-MgO catalytic sorbents due to its stronger capability on CH 3 OH activation and CO 2 adsorption.
研究领域:
催化化学
·
材料科学
·
能源化学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Qibin Zhu,Long Chen,Yun Da
The Calcium looping thermochemical reaction directly driven by solar energy effectively addresses the problem of efficient energy storage of concentrated solar power plants (CSP) by shortening the energy conversion path. But new requirements are put forward for energy storage materials, including high solar radiation absorption, high cycling stability and fast kinetics. To meet these challenges, we have designed porous microsphere structures for the purpose of enhancing mass transfer and the capture of solar radiation. Additionally, Zr and Mn oxides with elevated Tammann temperatures were incorporated to stabilize the morphology and prevent sintering. The synthesized porous microspheres retained abundant mesoporous channels on the surface even after undergoing 20 cycles. The addition of Mn oxide significantly enhances solar spectral absorptivity, achieving an impressive 82.88 % absorbance. The incorporation of Mn and Zr oxides increased the sintering resistance, specific surface area and porosity of CaO/CaCO 3 , especially in the 10–100 nm range, which accelerated the CO 2 transport during carbonation. These enhancements significantly improve the chemical control stage of the carbonation reaction, as further supported by kinetic models. After 50 cycle experiments at 800 °C, the energy storage density of the sample remains at 1074 kJ/kg, which is 1.86 times that of the undoped CaCO 3 . This study provides a new way to design CaCO 3 materials suitable for CSP applications.
研究领域:
材料科学
·
可再生能源
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2024
·
IF 5.5
Yuanyuan Tian,Hui Wang,Shengli Liu,Bo Zhang
Zirconium (Zr)-doped NiO films with different contents were successfully synthesized via the chemical spray pyrolysis technique. The structure, morphology, optical and electrochemical behaviors of these films were investigated by X-ray diffraction (XRD), Raman spectrometer, scanning electron microscopy (SEM), energy dispersive spectrometer (EDS), UV–Vis-NIR spectrophotometry, cyclic voltammetry (CV), and chronoamperometry (CA). XRD results suggested that the synthesized samples have the cubic crystal structure and a preferred orientation along the plane (111). Raman spectra further confirmed the successful incorporation of zirconium ions into the NiO films. SEM images explained that the surfaces of the doped films were composed of uniform and dense nanoparticles. EDS analysis suggested that Zr, Ni and O elements were uniformly distributed on the films. The optical results showed that the band gap decreases from 3.53 eV to 3.47 eV as the increase of zirconium doping content. The electrochemical analysis suggested that zirconium doping improved the specific capacitance of the NiO films (the NiO film with the Zr amount of 7 %, 59 F/g at 6 mV/s). In addition, the NiO film with 5 % Zr doped amount exhibited the largest Δ OD (81 %), the largest CE (60.37 cm 2 /C), and the fastest coloring time ( t c =2.1 s) and bleaching time ( t b = 2.4 s). These results showed that this film had the excellent electrochromic properties, suggesting that the optimal Zr doped amount of NiO films is 5 %. As a novel kind of electrochromic material, the Zr-doped NiO film has broad application prospects in smart windows, green buildings and energy efficient utilization fields.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Catalysts
·
2021
·Vol. 11
·期 6
·710
·
IF 4.146
Linmeng Huo,Tian Wang,Keng Xuan,Lei Li,Yanfeng Pu,Chenxin Li,Congzhen Qiao,Hao Yang,Yan Bai
The adsorption and activation of both CO2and methanol are mainly affected by the distance of the Lewis acid site, Zr4+, and Lewis base, Zr4+/O2−, of the Zr-based catalysts. In this paper, Zr-incorporated SBA-15 (Zr-SBA-15) and Zr-grafted SBA-15 (Zr/SBA-15) catalysts were prepared with different Zr environments, and were analyzed with N2adsorption–desorption isotherms, X-ray diffraction, UV-vis spectra, and XPS. It was proposed that Zr-SBA-15 catalyst with Si-O-Zr-OH and Zr-O-Si-OH structure exhibited non-adjacent sites between Zr4+and Zr4+/O2−, while Zr/SBA-15 catalyst with Zr-O-Zr-OH structure showed neighboring sites between Zr4+and Zr4+/O2−. Furthermore, the Zr/SBA-15 catalyst exhibited good catalytic activity, while no DMC was detected over the Zr-SBA-15 catalyst at the same reaction conditions. For combined in situ infrared and catalytic performance, it was indicated that the methanol and CO2could be activated to form DMC, only when the Zr4+and Zr4+/O2−sites existed and were adjacent to each other in the Zr-O-Zr-OH of Zr/SBA-15 catalyst.Keywords:dimethyl carbonate;in situ FTIR spectra;ZrO2-grafted SBA-15;Zr-incorporated SBA-15;carbon dioxide
研究领域:
催化化学
·
环境科学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）