WATER RESEARCH
·
2025
·
IF 12.4
Ziyi Zhao,Yanan Mi,Shili Wang,Xuedong Du,Qingrui Zhang
We firstly present a novel strategy for enhancing fluoride removal from contaminated water using defect-engineered UiO-66 (Zr-MOFs), emphasizing the crucial role of pKa in modulator selection. By utilizing modulators with varying pKa values-specifically benzimidazole (BI), benzoic acid (BA), and acetic acid (AA)-we synthesized defect-rich Act-UiO-66-M(X). The higher pKa of BI facilitated greater defect formation, resulting in significantly improved adsorption capacity and faster diffusion rates. Act-UiO-66-BI(8), modulated with BI, showed a higher intensity peak at g = 2.003 in ESR analysis, indicating more oxygen vacancies. Its fluoride adsorption capacity reached 93.59 mg F/g, nearly six times higher than commercial ZrO 2 , with rapid kinetics—evidenced by a kinetic rate constant (k int ) of 2.64 mg/g·min 0.5 and equilibrium achieved within 10 minutes. The kinetic performance was enhanced by 270% compared to raw Act-UiO-66. Furthermore, Act-UiO-66-BI(8) demonstrated high selectivity and stability in high-salinity environments, with a K d coefficient consistently exceeding 17,900 mL/g. The study highlights that selecting modulators based on pKa enhances defect formation, improving active site exposure and pore diffusion, as confirmed by DFT calculations and XPS analysis. The ability of Act-UiO-66-BI(8) to treat up to 1160 kg of wastewater per kg of adsorbent highlights its potential for large-scale water purification, showcasing a promising approach for developing high-performance MOF materials.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Mao Fu,Xuepeng Deng,Shi-Qiang Wang,Fenglin Yang,Li-Chiang Lin,Michael J. Zaworotko,Yingchao Dong
To find sustainable water solutions, the development of high capacity, scalable robust adsorbents and mechanistic insight about their performance offers the potential to effectively address the global challenges of water scarcity and water contamination. We herein rationally design Zr-cluster defective MOF-808 (MOF-808 def ) with exposed carboxyl groups, a robust zirconium metal–organic framework (Zr-MOF), exhibiting high adsorption capacity (q max ∼ 296 mg·g −1 ) coupled with high selectivitity for tetracycline (TC) antibiotics, outperforming other water-stable MOFs, commercial and inorganic nano-adsorbents. MOF-808 def functions well across a wide range of contaminant concentrations (from trace to high-concentration) and even in harsh conditions ( e.g. , high acidity and salinity). Both experimental and simulation results indicate that the mechanism of adsorption involves both physisorption and chemisorption via hydrogen bonding, electrostatic interactions (EIs) and C-O-C covalent bonding via esterification. Computational studies confirm that hydrogen bonding plays a key role in strong guest–host interactions between TCs and MOF-808 def . Further, defects resulting from missing-Zr-clusters in MOF-808 def are confirmed to enhance adsorption performance. Specifically, the defect sites present exposed carboxyl groups from MOF-808 def linker ligands that selectively react with –OH groups (phenol and tertiary alcohol moieties) in TC via esterification. These defects drive highly selective adsorption even at low concentrations of TCs ( e.g. , 500 ppb). Aiming for more than enhanced performance, economic estimation and scalable engineered reactor tests revealed that MOF-808 def and its nano-composites are free of environmental risks and offer promise for sustainable water treatment at pilot scale. The use of defect-engineering rationales is a molecule-level design concept that could be generally useful for the development of the next generation of MOF-based nano-adsorbents for sustainable water treatment applications.
研究领域:
材料科学
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环境科学
✓ 已验证
DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2021
·Vol. 168
·期 10
·103507
·
IF 4.316
Fuhua Chen,Hao Guo,Lili Zhao,Xin Guo,Shunchang Li,Ying Chu,Xueying Wang,Yongping Zhu
As a cathode material for thermal batteries, WS2 has high thermal decomposition temperature and large specific capacity, but it is an intermittent semiconductor, with relatively low conductivity. This low conductivity can prolong the activation time and reduce the discharge specific capacity of thermal batteries. Here, we prepared WS2 with sulfur vacancies through a simple high-temperature annealing method and used electron paramagnetic resonance spectroscopy and X-ray photoelectron spectroscopy to detect the presence of sulfur vacancies. The result shows that sulfur vacancies were successfully introduced in WS2, and the existence of sulfur vacancies can effectively improve the discharge performance of thermal batteries. While maintaining the nanostructure, the thermal decomposition temperature still exceeds 1000 °C, which is far beyond the traditional FeS2 (550 °C) and CoS2 (650 °C) cathodes. The Li-B/LiF-LiBr-LiCl/WS2 with sulfur vacancies (treated at 500 °C) couple has higher discharge specific capacity (when the cut-off voltage is 0.5 V, it is 380.58 mAh g−1, which is 14.85% higher than the original WS2) and lower total polarization (about 21% lower than original WS2). This work provides a beginning for further study of sulfur vacancies defect materials as the cathode of thermal batteries.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
You Xu,Kaili Ren,Tianlun Ren,Mingzhen Wang,Ziqiang Wang,Xiaonian Li,Liang Wang,Hongjing Wang
Electrochemical reduction of nitrate (NO 3 - ) to ammonia (NH 3 ) offers a sustainable avenue to close the NO 3 - cycle for NH 3 synthesis. Critical to the feasibility of electrochemical NO 3 - -to-NH 3 technology is the development of cost-effective, scalable and selective catalysts that can produce NH 3 with high yield. To this end, we design and constructure ultralow-content Pd (2.93 at%) in-situ incorporated Cu 2 O corner-etched octahedra (Pd-Cu 2 O CEO) with cavity and oxygen vacancy defects for selectively electrochemical NO 3 - -to-NH 3 transformation. The unique conner-etched cavity structure, rich surface oxygen vacancies, and Pd-Cu 2 O dual active sites, synergistically promote nitrate electroreduction undergo ammonia formation reaction pathway. Impressively, the as-made Pd-Cu 2 O CEO exhibited outstanding activity for electrocatalytic NO 3 - -to-NH 3 , with high ammonia selectivity (95.31%) and Faradaic efficiency (96.56%). The developed hierarchical-defect strategy may open a new avenue for reasonable design of defect electrocatalysts to contribute desirable properties and functionalities in specific applications.
研究领域:
电化学催化
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Fei Fang,Quankun Lv,Peng Li,Yue Tao,Yan Zhang,Yi Zhou,Xuede Li,Jie Li
Defect engineering is essential for improving the adsorption performance of metal-organic frameworks (MOFs). Herein, hierarchical porous UiO-67(Zr) and analogs with controlled levels of defects were successfully obtained and applied to chemoselectively capture glyphosate (GP) from water. The obtained defective UiO-67 was stable at different pH values. The removal performance of defective UiO-67(Zr) was evaluated systematically as a function of different modulators, water chemistry and interfering ions. The maximum adsorption capacity of defective UiO-67(Zr) reached 322.58 mg/g, superior to most MOFs-based adsorbents. The defective UiO-67(Zr) also showed high selectivity for GP adsorption at high concentrations of humic acids (3 times) and interfering anions (100 times). In addition, the defective UiO-67(Zr) has shown good recovery performance and can effectively remove GP from a variety of contaminated water samples and multi-pollutant systems. The results of batch experiments and microscopic spectral characterization (XPS and FTIR) revealed that GP adsorption was mainly guided by electrostatic action, coordination, pore-filling and hydrogen bonding . These findings verified that the fabrication of defect sites played an important role in promoting the adsorption performance of MOFs. Our work provides a clue to the design of defective MOFs with high adsorption performance.
研究领域:
环境科学
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材料科学
✓ 已验证
DOI
高影响因子
ANALYTICAL CHEMISTRY
·
2022
·
IF 8.008
Jing Lei,Wei Liu,Yan Jin,Baoxin Li
Defect engineering is an effective strategy to improve the catalytic activity of metal oxides, and quantitative characterization of surface defects is thus vital to the understanding and application of metal oxide catalysts. Herein, we found that ZnO nanoparticles with oxygen vacancy could trigger the luminol–H2O2 system to emit a strong chemiluminescence (CL), and the CL intensity was strongly dependent on the oxygen vacancy of the ZnO nanoparticles. The mechanism of this CL reaction was discussed by means of the electron-spin resonance spectrum, X-ray photoelectron spectrum (XPS), and CL spectrum. The oxygen vacancy-dependent CL was attributed to the ability of the oxygen vacancy to readily adsorb and further dissociate H2O2 into active •OH radicals. Taking advantage of this oxygen vacancy-dependent CL, we presented one method for quantifying the oxygen defects in ZnO. Compared with the current evaluation techniques (XPS and Raman spectroscopy), this CL method is rapid, low-cost, and easy to operate. This work introduces the CL technique into the field of material structure–property evaluation, and provides a new approach for exploring the defect function in ZnO defect engineering.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACTA MATERIALIA
·
2023
·
IF 9.4
Siyu Wang,Ning Ding,Dandan Han,Ping Wang,Yupeng Dang,Pengcheng Xu,Yanwei Sui,Yen Wei
Defects in nanomaterials have been widely used to introduce new properties of pristine materials for electrochemical energy storage. However, most of the research has focused on the effect of single defect while ignoring the synergy of multifold defects on enhancing electrochemical performance . Herein, we have modeled bulk phase oxygen substitution and surface oxygen vacancy on ZnCo 2 O 4 nanowires grown on nickel foam for the first time (F-ZnCo 2 O 4-x ), revealing the role of double defects and providing new insights into the effects of electrochemical properties . The enhanced oxygen vacancy concentration and increased active sites enable rapid and sufficient redox reaction of the active components. Therefore, the representative F-ZnCo 2 O 4-x electrode achieves a high specific capacity of 664 mAh·g −1 at 1 A·g −1 . Moreover, high energy density (E HSC , 60 Wh·kg −1 ) and good cycle stability (90.44% capacity retention after 10000 cycles) could be provided as a battery-type electrode of hybrid supercapacitor . The electrodes also have high energy density (E cell , 692 Wh·kg −1 ) and good durability (capacity retention of 98.8% after 2000 cycles) when used as zinc ion batteries . This work supplies a new avenue on the universality of defect engineering to design bimetallic oxide with high electrochemical performance .
研究领域:
材料科学
·
电化学能源存储
✓ 已验证
产品关联
DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2025
·
IF 7.7
Baoshuai Xing,Xiaoli Cheng,Tingting Wang,Xianfa Zhang,Lihua Huo,Yingming Xu
Chlorine (Cl 2 ) is a highly hazardous and corrosive substance that can cause severe respiratory problems and skin burns in humans at low doses. The effective detection of Cl 2 has become critical for protecting both the ecological environment and public health. Herein, the oxygen vacancy-abundant SnO 2 were synthesized using SnS as template followed by the calcination method. The resultant SnO 2 -800 sensor exhibits improved sensing response to Cl 2 (about 205–10 ppm) at room temperature, together with a trace detection limit of 100 ppb. Such excellent sensing properties could be assigned to several reasons including the unique cross-linked structure, the appropriate amount of grain boundaries, and especially sufficient oxygen vacancies. The XPS, GC-MS techniques and DFT theoretical calculation were combined used to detailly investigate the sensing mechanism. This work might shed light on the rational design of high-performance sensing materials via defect engineering.
研究领域:
材料科学
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环境科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
CERAMICS INTERNATIONAL
·
2025
·
IF 5.6
Ziheng Wei,Yongping Liu,Qi Ding,Yuena Zhang,Yu Ren,Jihu Chen,Mingming Si,Yuchi Fan,Wan Jiang
Conductive two-dimensional (2D) materials exhibit excellent electromagnetic wave (EMW) absorption properties at high frequencies due to their high conductivity loss. However, their unsatisfactory EMW absorption at low frequencies, attributed to impedance mismatch, remains a significant challenge. In this work, high-conductivity 1T′ WTe 2 nanosheets were incorporated into insulating mesoporous channels of Santa Barbara Amorphous-15 (SBA-15) via chemical vapor deposition (CVD), resulting in the formation of 1T′ WTe 2 /SBA-15 composites. These mesoporous channels restrict the growth of 1T′ WTe 2 and hinder carrier migration cross the channels, reducing their conductivity. Meanwhile, heterogeneous interfaces were formed between 1T′ WTe 2 nanosheets and mesoporous channels of SBA-15, accompanied by defects within the 1T′ WTe 2 nanosheets. This interaction promotes dipole polarization losses, significantly enhancing the attenuation of incident EMW, particularly at low frequencies. Consequently, the effective absorption bandwidth (EAB) of 1T’ WTe 2 /SBA-15 composites within the S band reached to 0.72 GHz, ranging from 3.28 GHz to 4.0 GHz, with a minimum reflection loss (RL min ) of −26.5 dB at 3.68 GHz. Furthermore, the EAB of the composites extended to 3.92 GHz at 1.5 mm in the high-frequency range. This work introduces a novel strategy for enhancing EMW absorption performance in the S band through heterogeneous interfaces and defect engineering, driven by the limiting effects of mesoporous channels.
研究领域:
材料科学
·
电子工程
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Mingxin Zheng,Keng Xuan,Shuai Yan,Yaoping Guo,Yaxiong Huang,Runling Xu,Kaixuan Zhao,Zebing Li,Xun Li,Hao Jiang,Yadan Guo
A defective metal–organic framework UiO-66–18 synthesized via a facile solvothermal synthesis method with trifluoroacetic acid as modulator was demonstrated to be highly efficient for the elimination of uranium from wastewater. The maximum adsorption capacity of UiO-66–18 toward uranium reached 622.75 mg g −1 , which was approximately 1.43 times higher than that of pristine UiO-66–0 prepared without TFA modulation. The superior elimination performance of UiO-66–18 was because the TFA modulation induced the generation of more missing-linker defects that endowed UiO-66–18 with hierarchical structure and more adsorption active sites for U(VI) capture. Further adsorption mechanism studies indicated that the elimination of U(VI) was endothermic monolayer chemisorption dominated by mass transfer-decomplexation-adsorption process. In addition, the effects of common ions on the elimination efficiency as well as the reusability of UiO-66–0 and UiO-66–18 were studied. This work provides a promising strategy and a theoretical basis for the design and preparation of efficient uranium adsorbent from the points of defects engineering and pore structure design.
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
CERAMICS INTERNATIONAL
·
2024
·
IF 5.1
Yiling Huang,Zeyu Chen,Yifei Xiong,jiajie Wu,Chucheng Lin,Wei Zheng,Caifen Jiang,Yi Zeng
Rare earth X2-type monosilicates with low thermal conductivity are crucial for material performance in extreme environments. Three high-entropy ceramics, (Er 1/4 Tm 1/4 Yb 1/4 Lu 1/4 ) 2 SiO 5 , (Y 1/4 Er 1/4 Tm 1/4 Yb 1/4 ) 2 SiO 5 , and (Gd 1/4 Dy 1/4 Er 1/4 Yb 1/4 ) 2 SiO 5 , were synthesized in this study. Among these, the thermal conductivity of (Y 1/4 Er 1/4 Tm 1/4 Yb 1/4 ) 2 SiO 5 at 1200 °C is 1.03 W m −1 K −1 . Concurrently, the stable existence of dislocation arrays was observed in the quaternary high-entropy monosilicate system of (Y 1/4 Er 1/4 Tm 1/4 Yb 1/4 ) 2 SiO 5 . The scattering of medium-frequency phonons can be enhanced by the presence of dislocations, leading to a reduction in thermal conductivity. This provides direct experimental evidence supporting the feasibility of reducing material thermal conductivity through high-entropy design by introducing dislocations.
研究领域:
材料科学
·
热物理
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Sihan Ma,Xian Luo,Guang Ran,Yipeng Li,Ziqi Cao,Xinyi Liu,Guoqiang Chen,Jianghua Yan,Lin Wang
Optical antibacterial agents present great potential in eliminating infectious pathogens. It is of great significance to construct effective photonic antibacterial agents with outstanding light absorption properties. Herein, 2D engineering defect nanosheets BiOI/Bi with Bi decoration and defect engineering (BiOI-DE) are constructed to perform photonic sterilization. On the one hand, the rational designed BiOI-DE can effectively promote the broad-spectrum light absorption ability to enhance the light utilization rate. On the other hand, the substantive structure can simultaneously harvest the enhanced photonic carriers and thermal effect when irradiated with high penetration ability NIR, further exhibiting higher activity in killing Escherichia coli (E. coli) than that of single BiOI with poor light absorption. The sterilization efficiency is over 99%. Moreover, the causes of the photothermal effect are discussed, indicating that the change of BiOI bandgap and surface bismuth decoration displays a critical role in enhancing light absorption and creating heat energy. In the meantime, the structural advancement of BiOI-DE effectively improves the photocatalytic activity, the synergistic photothermal-catalytic process establishes a favorable condition for improving antibacterial performance. This system provides rational design and potential inspiration for high efficient antibacterial strategy by employing defect engineering approaches.
研究领域:
材料科学
·
生物医学
·
光催化
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）