Journal of Materials Chemistry A
·
2024
·
IF 10.7
Ling-Xia Yun,Meng Qiao,Bin Zhang,Hang-Tian Zhang,Jie-Xin Wang
Utilizing plastic wastes as linker sources for metal–organic framework (MOF) synthesis is a green and sustainable methodology for the chemical upcycling of plastics. However, improving the depolymerization efficiency of polymers and avoiding highly corrosive solvents during the purification of the products remain significant challenges. Herein, we propose an approach to efficiently hydrolyze practical poly(ethylene terephthalate) (PET) wastes using aqueous dispersions of ultrasmall ZnO (6 nm) nanoparticles as the catalysts and subsequently synthesize five typical nano-MOFs by one-pot and two-pot strategies. The neutral hydrolysis of PET is greatly accelerated, with PET being completely depolymerized at 200 °C in 60 min with a terephthalic acid yield of 95.6%. The PET-derived MOF nanoparticles present high BET surface areas that are higher than or close to those of congeneric MOFs synthesized from petroleum-based and highly purified ligands. As a water absorbent, the two-pot MIL-101(Cr) exhibits high thermal stability with a water uptake capacity of 1327.3 mg g−1. For photocatalytic degradation of antibiotic pollutants, MIL-53(Al, Fe) samples derived from PET textiles show a high tetracycline removal efficiency of over 90% within 60 min without additives in an aqueous system, outperforming most of the conventionally prepared MOF catalysts. This approach disposes of discarded plastics in an eco-friendly way and produces value-added materials with excellent catalysis and adsorption properties.
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Sheng Liao,Shunli Shi,Jie Hu,Yunpeng Zeng,Weiming Xiao,Shuhua Wang,Chao Chen
Hydrogen production through water electrolysis is a crucial method for generating hydrogen; however, the oxygen evolution reaction (OER) requires high reaction potentials, leading to significant electrical energy consumption. In contrast, aldehyde oxidation at ultra-low potentials offers a promising alternative to OER. Coupling aldehyde oxidation with the hydrogen evolution reaction (HER) forms an ideal system for hydrogen production, simultaneously generating high value-added oxidation products and avoiding less economically valuable O 2 . This study employs a photoelectrocatalytic system to drive the oxidation of formalin solutions in a safe and sustainable manner. Utilizing water as the oxidant, the system provides a viable strategy for dual hydrogen production and organic synthesis in neutral media. Under an applied bias voltage of 0.6 V vs. Ag/AgCl and simulated sunlight of 100 mW cm −2 , the BiVO 4 photoanode achieved 83% selectivity for formic acid production. Furthermore, dual hydrogen production was realized at both the anode and cathode, with an apparent Faradaic efficiency of 35%. This work presents an energy-saving and environmentally friendly pathway for solar hydrogen storage and the production of high value-added chemicals, underscoring the potential application of the photoelectrochemical (PEC) method in coupled systems.
研究领域:
能源科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
Nano-Micro Letters
·
2020
·Vol. 12
·期 1
·1-16
·
IF 12.264
Zhang Shucong,Wang Wenbin,Hu Feilong,Mi Yan,Wang Shuzhe,Liu Youwen,Ai Xiaomeng,Fang Jiakun,Li Huiqiao,Zhai Tianyou
The 2D CoOOH sheet-encapsulated Ni 2 P into tubular arrays electrocatalytic system with expediting mass transport, structural stability, and tuned electron was conceptually proposed.
The designed electrocatalysts realize expectant 1000 mA cm −2 -level-current-density hydrogen evolution in neutral water for over 100 h.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Hossain M. Shahadat,Nazir Ahmad,Zafar A.K. Khattak,Rahaman M. Abdur,Rashid Al-Hajri,Mohammed Al-Abri,Chih-Ming Kao,Hussein A. Younus,Francis Verpoort
Hydrogen (H 2 ) production via water splitting under completely aqueous conditions particularly using an earth-abundant component for both half reactions is very appealing and may reduce our dependence on fossil fuels. In this work, we present a water-soluble molecular nickel(II) complex bearing a macrocyclic N ‒heterocyclic carbene (NHC)/pyridine hybrid ligand, ([NiL](PF 6 ) 2 (L = bis(2‒pyridyl-methylimidazolylidene)methane as a catalyst for hydrogen evolution reaction (HER) under completely aqueous conditions. The catalyst displayed an outstanding catalytic activity for HER in a phosphate electrolyte of neutral pH, as established by a series of techniques. Long-term (11 h) bulk electrolysis at 0.88 V overpotential provides a maximum of 173.5C charge and total ca . 165.08 μmol (∼15 μmol per hour) H 2 with Faradaic efficiency of 98%, while without a catalyst less than 3C was produced within the same time. To the best of our knowledge, the investigation of water reduction with Ni–NHC type catalyst under aqueous conditions has not been reported to date.
研究领域:
化学
·
能源科学
✓ 已验证
DOI
高影响因子
ChemElectroChem
·
2024
·Vol. 11
·期 10
·e202300710
·
IF 3.5
Hussein A. Younus,Heba Emam,Nazir Ahmad,Mosaad Negm,Muneerah Alomar,Fatma M. Elantabli,Mohammed M. El-Rabiei,Rashid Al Hajri,Shiguo Zhang,Mohammed Al Abri
Graphical Copper Glycine Schiff Base Catalyst : Mimicking natural processes, this dinuclear copper catalyst with a Schiff base ligand efficiently catalyzes HER from neutral water, showcasing remarkable rate and stability. It reaches ~19 mA cm −2 at −0.7 V vs. RHE ( i c /i p =166), corresponding to a k obs of ~27,000 s −1 , one of the highest TOFs for an earth-abundant molecular catalyst under similar coditions. The development of an efficient and stable electrocatalyst for the hydrogen evolution reaction (HER), based on earth-abundant components, represents a crucial step toward cost-effective and environmentally friendly hydrogen production. This study presents the utilization of a dinuclear copper catalyst, denoted as [Cu-Gly-SB] (Complex 1 ), for HER under both aqueous and non-aqueous conditions. In non-aqueous settings, the catalyst achieves excellent HER performance, requiring only a 270 mV overpotential when acetic acid is used as the proton donor. Notably, in fully aqueous conditions, complex 1 attains a remarkable current density of 18.8 mA ⋅ cm −2 at −0.7 V vs . RHE in cyclic voltammetry. The k obs value of ≈2.7×10 4 s −1 in aqueous solution at pH 7.0 further underlines the superior catalytic performance of 1 , outperforming most non-noble-metal molecular catalysts functioning in fully aqueous solutions. The robust stability of 1 is demonstrated through controlled potential electrolysis (CPE) over a span of 48 hours, achieving an impressive catalytic current of 11.0 mA ⋅ cm −2 at −0.39 V. Moreover, the catalytic current gradually increases with higher reduction potentials, reaching a substantial 100 mA ⋅ cm −2 at an overpotential of 590 mV during CPE >48 hours. Thorough characterizations further confirm the molecular nature of the catalyst.
研究领域:
化学
·
材料科学
·
催化科学
✓ 已验证
DOI
高影响因子
International Journal of Minerals Metallurgy and Materials
·
2020
·Vol. 27
·期 2
·220-231
·
IF 1.713
Yang Tao,Liu Hui-juan,Bai Fan,Wang En-hui,Chen Jun-hong,Chou Kuo-Chih,Hou Xin-mei
Currently, developing supercapacitors with robust cycle stability and suitability for wide-temperature-range operations is still a huge challenge. In the present work, few-layer hexagonal boron nitride nanosheets (h-BNNSs) with a thickness of 2–4 atomic layers were fabricated via vacuum freeze-drying and nitridation. Then, the h-BNNSs/reduced graphene oxide (rGO) composite were further prepared using a hydrothermal method. Due to the combination of two two-dimensional (2D) van der Waals-bonded materials, the as-prepared h-BNNSs/rGO electrode exhibited robustness to wide-temperature-range operations from −10 to 50°C. When the electrodes worked in a neutral aqueous electrolyte (1 M Na 2 SO 4 ), they showed a great stable cycling performance with almost 107% reservation of the initial capacitance at 0°C and 111% at 50°C for 5000 charge—discharge cycles.
研究领域:
材料科学
·
能源存储技术
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2024
·
IF 8.4
Shiqi Peng,Li Gao,Xiaobin Jiang,Xuehua Ruan,Xuemei Wu,Xiaopeng Zhang,Xiaoming Yan,Gaohong He
Neutral aqueous organic redox flow battery (NAORFB) represents a highly promising energy storage device. However, one of its challenges is the need for high Cl − conductivity, highly stable ion-selective membranes. In this work, N-methylpiperidine-modified carbazole-based long side chain anion exchange membranes (QPCEP-x) were designed and prepared. The rigidity and hydrophobicity provided by the carbazole on the main chain, in conjunction with the flexibility and hydrophilicity provided by the alkyl-piperidine groups on the side chains, resulted in the observed excellent microphase separation properties of the prepared membranes. The prepared membranes exhibited excellent overall performance, with QPCEP-1 achieving a Cl − conductivity of 20.33 mS cm −1 at 25 °C. In NAORFB, the energy efficiency of QPCEP-1 ranges from 91.7 % to 62.4 % at 20–160 mA cm −2 , far exceeding the 89.1 %–38.4 % of commercial AMVN. Furthermore, long-term cell cycling tests demonstrate that the energy efficiency of QPCEP-1 remains unchanged at 82.7 % at 60 mA cm −2 after 10,000 complete charge and discharge cycles, exceeding the majority of cycles reported in literatures. These findings suggest that QPCEP-x has significant potential for use in NAORFB.
研究领域:
材料科学
·
能源存储技术
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2019
·Vol. 7
·期 39
·22453-22462
·
IF 10.733
Liang Yan,Bing Zhang,Junlu Zhu,Zhonggang Liu,Haiyan Zhang,Yunyong Li
Exploring highly efficient and cost-effective electrocatalysts has become imperative for neutral-pH water splitting, which is environmentally friendly and can reduce the cost of electrolysis systems. Here, we report an effective strategy to design a novel type of callistemon-like Zn and S codoped CoP nanorod clusters by introducing both Zn and S into cobalt phosphide, thereby creating electrocatalysts for highly efficient and stable neutral water splitting. The best Zn and S codoped CoP nanorod clusters on carbon paper (Zn,S–CoP NRCs/CP) require overpotential values of 67 and 391 mV for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) at 10 mA cm−2 in 1.0 M phosphate-buffered solution, respectively. Remarkably, this enables a neutral electrolyzer to deliver 10 mA cm−2 at a low cell voltage of 1.70 V, which is superior to those afforded by the Pt/C/CP‖IrO2/CP couple and most of the state-of-the-art electrocatalysts. Impressively, this electrolyzer can be powered by an AA battery (∼1.5 V). Density functional theory computations and systematic experiments have verified that the improved HER and OER activities originate from the optimized electronic structures that can facilitate the adsorption and desorption of hydrogen intermediates after introducing Zn and S and accelerating the formation of oxygenated intermediates on CoOOH, respectively. This work provides a new strategy to boost the performance of transition metal phosphides for neutral water or seawater splitting.
研究领域:
材料科学
·
能源化学
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2022
·
IF 10.53
Yan Xiao,Junhui Xu,Lei Hu,Hui Wang,Li Gao,Shiqi Peng,Mengting Di,Xiaojun Sun,Jie Liu,Xiaoming Yan,Liuping Chen,Gaohong He
Neutral aqueous organic redox flow battery (NAORFB) stands out as one of the most prospective mass energy storage options. The main limitations of large-scale storage regarding the NAORFB lie in the low Na + /Cl − conductivity of membrane in pH7 systems, which leads to a lower voltage efficiency. Herein, quaternary ammonium functionalized fluorinated poly (arylene ether) (QAFPAE-x) anion exchange membrane with hydrophilic and hydrophobic blocks was designed successfully. The results demonstrated that the grafting of quaternary ammonium and fluorine-containing block enables QAFPAE-x membrane low swelling, high Cl − conductivity, and promising chemical stability characteristics. The voltage efficiency of QAFPAE-100 membrane (93.8%–60.7%) is much higher than the AMVN membrane (88.4%–37.8%) at 20–160 mA cm −2 . Furthermore, the NAORFB with the QAFPAE-100 membrane steadily runs at 60 mA cm −2 over 1500 cycles. Therefore, the ionic highway induced excellent performance of QAFPAE-100 membrane to render this material a promising candidate for practical NAORFB applications.
研究领域:
材料科学
·
能源存储
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
CERAMICS INTERNATIONAL
·
2021
·
IF 4.527
Jun Ping,Sajid Rauf,Zuhra Tayyab,Changping Yang
Layer-structured lithium cobalt oxide (LCO) is one of promising electrode materials for secondary aqueous lithium-ion batteries, yet the effect of structural proton insertion in LCO in neutral aqueous electrolytes cannot be ignored. Present study investigates the electrochemical performance of polycrystalline spherical LCO in neutral aqueous saturated Li 2 SO 4 solution. Herein, we for the first time demonstrate the dependence of LCO stability on the discharge cutoff potential. The applied LCO electrodes show good cycling stability within the potential window of 0.65–1.1 V vs. SCE, while electrochemical impedance spectrum (EIS) analysis detects no sign of proton intercalation. Moreover, the spherical LCO free from the proton intercalation exhibits a superior rate capability with 78% discharge capacity retention at 80 C. The lithium-ion chemical diffusion coefficient being seven times than that of irregular shaped LCO sample can be responsible for such significant rate capability. The cyclability testing depicts the better performance of spherical LCO in comparison with the counterpart, especially in terms of electrode activation time. Post cycling electrode characterization displays that the discharge capacity fading of LCO mainly results from the crystal grain deformation due to high potential cycling and can be alleviated by reducing the depth of charge.
研究领域:
材料科学
·
电化学
·
电池技术
✓ 已验证
DOI
高影响因子
Science Bulletin
·
2025
·
IF 21.1
Xiangcheng Zhang,Silian Cheng,Xue Wen,Weiyao Hu,Ziyi Chen,Hongshuai Cao,Panzhe Qiao,Xue Li,Lizhi Zhang,Mingce Long
Hydrogen peroxide (H 2 O 2 ) photosynthesis from H 2 O and O 2 remains a significant challenge due to the sluggish hydrogen donation process, which stems from the high O–H bond dissociation energy of water. In this study, we propose an effective strategy to accelerate the water oxidation reaction (WOR) by anchoring single palladium atoms (Pd–CNO 2 ) onto a keto-anthraquinone covalent organic framework (KfAQ-Pd), achieving remarkable H 2 O 2 production rates of 3828 μmol h −1 g −1 under visible light irradiation ( λ > 420 nm) in neutral water. Both experimental observations and theoretical simulations reveal that the Pd–CNO 2 configuration induces an upward shift in the d-band center and enhances the hydrophilicity of KfAQ. This modification effectively disrupts the hydrogen-bond network within adsorbed water clusters, thereby promoting the cleavage of the dangling O–H bonds in H 2 O molecules and facilitating efficient hydrogen donation. The generated H 3 O + species are subsequently reduced in-situ by photogenerated electrons, leading to the hydrogenation of anthraquinone moieties and ultimately driving efficient H 2 O 2 photosynthesis. Overall, these findings highlight the pivotal role of single Pd atoms in enhancing water dissociation and hydrogen transfer, offering a promising new paradigm for solar-driven, environmentally friendly H 2 O 2 synthesis in neutral aqueous systems.
研究领域:
材料科学
·
光催化
·
可持续能源
·
环境化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
FOOD CHEMISTRY
·
2023
·
IF 8.8
Haolin Zhang,Shiye Lin,Ruiwei Xie,Weizhi Zhong,Hui Wang,Mohamed A. Farag,Hidayat Hussain,Randolph R.J. Arroo,Xiaojia Chen,Jianbo Xiao
In the field of thermal degradation of flavonoids, current studies mainly focused on flavonols. However, the thermal degradation of dihydroflavonols in aqueous solution has received limited attention compared to flavonols. The single C2-C3 bonds of dihydroflavonols, which differs from the C2-C3 double bond in flavonols, may cause different degradation mechanisms. Dihydromyricetin (DMY) is a typical dihydroflavonol with six hydroxyl groups, and possesses various health effects. We explored the thermal degradation of DMY in neutral aqueous solution (pH 7) at 100 ℃. Ultra-performance liquid chromatography combined with photodiode array and electrospray ionization quadrupole-time-of-flight tandem mass spectrometric detection (UPLC-PDA-ESI-QTOF–MS/MS) provided suitable platform for exploring DMY degradation pathways, and negative ion mode was applied. Thermal treatment led to a decline in DMY level with time, accompanied by the appearance of various degradation products of DMY. Degradation mechanisms of DMY included isomerization, oxidation, hydroxylation, dimerization and ring cleavage. The pyrogallol-type ring B of DMY might be initially oxidized into ortho -quinone, which could further attack another DMY to form dimers. In addition, hydroxylation is likely to occur at C-2, C-3 of DMY or DMY dimers, which then further yields ring-cleavage products via breakage of the O1-C2 bond, C2-C3 bond, or C3-C4 bond. The 3-hydroxy-5-(3,3,5,7-tetrahydroxy-4-oxochroman-2-yl) cyclohexa-3,5-diene-1, 2-dione ( m / z 333.0244) and unknown compound m / z 435.0925 were annotated as key intermediates in DMY degradation. Four phenolic acids, including 3,4,5-trihydroxybenzoic acid ( m / z 169.0136, RT 1.4 min), 2,4,6-trihydroxyphenylglyoxylic acid ( m / z 197.0084, RT 1.7 min), 2-oxo-2-(2,4,6-trihydroxyphenyl) acetaldehyde ( m / z 181.0132, RT 2.4 min), and 2,4,6-trihydroxybenzoic acid ( m / z 169.0139, RT 2.5 min) were identified as the major end products of DMY degradation. In addition, 5-((3,5dihydroxyphenoxy) methyl)-3-hydroxycyclohexa-3,5-diene-1,2-dione (m / z 261.0399, RT 11.7 min) and unidentified compound with m / z 329.0507 (RT 1.0 min) were also suggested to be end products of DMY degradation. These results provide novel insights on DMY stability and degradation products. Moreover, the heat treatment of DMY aqueous solution was found to gradually reduce the antioxidant activities of DMY, and even destroy the beneficial effect of DMY on the gut microbiota composition.
研究领域:
药学化学
·
分析化学
·
食品科学
·
药理学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）