JOURNAL OF ENVIRONMENTAL MANAGEMENT
·
2024
·
IF 8
Xuelian Xia,Xu Han,Yuanzheng Zhai
In aquifers, the sequestration and transformation of organic carbon are closely associated with soil iron oxides and can facilitate the release of iron ions from iron oxide minerals. There is a strong interaction between dissolved organic matter (DOM) and iron oxide minerals in aquifers, but the extent to which iron is activated by DOM exposure to active iron minerals in natural aquifers, the microscopic distribution of minerals on the surface, and the mechanisms involved in DOM molecular transformation are currently unclear. This study investigated the nonbiological reduction transformation and coupled adsorption of iron oxide minerals in aquifers containing DOM from both macro- and micro perspectives. The results of macroscopic dynamics experiments indicate that DOM can mediate soluble iron release during the reduction of iron oxide minerals, that pH strongly affects DOM removal, and that DOM is more efficiently degraded at low rather than high pH values, suggesting that a low pH is conducive to DOM adsorption and oxidation. Spherical aberration-corrected scanning transmission electron microscopy (SACTS) indicates that the reacted mineral surfaces are covered with large amounts of carbon and that dynamic agglomeration of iron, carbon, and oxygen occurs. At the nanoscale, three forms of DOM are found in the mineral surface agglomerates (on the surfaces, inside the surface agglomerates, and in the polymer pores). The microscopic organic carbon and iron mineral reaction patterns can form through oxidation reactions and selective adsorption effects. Fourier transform ion cyclotron resonance mass spectra indicate that both synergistic and antagonistic reactions occur between DOM and the minerals, that the release of iron is accompanied by DOM decomposition and humification, that large oxygen- and carbon-containing molecules are broken down into smaller oxygen- and carbon-containing compounds and that more molecules are produced through oxidation under acidic rather than alkaline conditions. These molecules provide adsorption sites for sediment, meaning that more iron can be released. Microscopic evidence for the release of iron was acquired. These results improve the understanding of the geochemical processes affecting iron in groundwater, the nonbiological transformation mechanisms that occur at the interfaces between natural iron minerals and organic matter, groundwater pollution control, and the environmental behavior of pollutants.
研究领域:
环境科学
·
地质学
·
化学
✓ 已验证
DOI
PubMed
高影响因子
Energy Storage Materials
·
2018
·
IF 0
Qian Liang,Fuming Chen,Shaofeng Wang,Qiang Ru,Qinyu He,Xianhua Hou,Ching-yuan Su,Yumeng Shi
Renewable energy-related technologies have become more important due to the increasing energy consumption. Herein, we put forward a novel organic flow desalination battery (ORFDB) using redox-active organic molecule electrolyte materials dissolved in the aqueous sodium chloride feed. Riboflavin-5’-phosphate sodium salt dihydrate (FMN-Na) is used as the anolyte, and the catholyte is 4-hydroxy-2,2,6,6-tetramethylpiperidin-1-oxyl (TEMPO). Sodium and chloride ions in salt feed were moved respectively to anolyte and catholyte by electrochemical reaction of electrolytes during the charge process, and return to the feed during the discharge process. This ORFDB system possesses the stable stability up to fifty cycles and the excellent rate performance. This ORFDB exhibits the cost-effective renewable energy storage and the possibility of salt removal based on the electrochemistry of organic molecules.
研究领域:
能源科学
·
电化学
·
材料科学
✓ 已验证
产品关联
DOI
Energy Material Advances
·
2021
·
IF 0
Shuzhi Hu,Liwen Wang,Xianzhi Yuan,Zhipeng Xiang,Mingbao Huang,Peng Luo,Yufeng Liu,Zhiyong Fu,Zhenxing Liang
A novel electroactive organic molecule, viz., 1-(1-oxyl-2,2,6,6-tetramethylpiperidin-4-yl)-1′-(3-(trimethylammonio)propyl)-4,4′-bipyridinium trichloride ((TPABPy)Cl3), is synthesized by decorating 2,2,6,6-tetramethylpiperidin-1-oxyl (TEMPO) with viologen, which is used as the positive electrolyte in neutral aqueous redox flow battery (ARFB). Extensive characterizations are performed to investigate the composition/structure and the electrochemical behavior, revealing the favorable effect of introducing the cationic viologen group on the electroactive TEMPO. Salient findings are as follows. First, the redox potential is elevated from +0.745 V for TEMPO to +0.967 V for decorated TEMPO, favoring its use as the positive electrolyte. Such an elevation originates from the electron-withdrawing effect of the viologen unit, as evidenced by the nuclear magnetic resonance and single crystal structure analysis. Second, linear sweep voltammetry reveals that the diffusion coefficient is 2.97×10−6 cm2 s−1, and the rate constant of the one-electron transfer process is 7.50×10−2 cm s−1. The two values are sufficiently high as to ensure low concentration and kinetics polarization losses during the battery operation. Third, the permeability through anion-exchange membrane is as low as 1.80×10−11 cm2 s−1. It is understandable as the positive-charged viologen unit prevents the molecule from permeating through the anion exchange membrane by the Donnan effect. Fourth, the ionic nature features a decent conductivity and thus eliminates the use of additional supporting electrolyte. Finally, a flow battery is operated with 1.50 M (TPABPy)Cl3 as the positive electrolyte, which affords a high energy density of 19.0 Wh L-1 and a stable cycling performance with capacity retention of 99.98% per cycle.
研究领域:
化学
·
能源科学
✓ 已验证
DOI
Nature Sustainability
·
2024
·
IF 25.7
Zhao Ziming,Li Tianyu,Zhang Changkun,Zhang Mengqi,Li Shenghai,Li Xianfeng
The growing global capacity for renewable energy generation necessitates the deployment of energy storage technologies with a combination of low cost, good performance and scalability. With these advantages, aqueous organic flow batteries have the potential to be the system of choice because they could store energy from organic redox-active molecules. Here we report naphthalene derivatives as organic redox-active molecules that exhibit high solubility (~1.5 M) and a stable redox-active framework with no obvious capacity decay over 40 days (50 Ah l −1 ) in an air atmosphere in flow batteries. We report a battery that runs smoothly even under continuous airflow without obvious capacity decay for ~22 days (more than 600 cycles). A series of spectral analyses and theoretical calculations reveal that the dimethylamine scaffolds improve the water solubility and protect the active centre, ensuring the stability of the molecules during the charge and discharge process. Owing to the success in kilogramme-scale molecular synthesis, pilot-scale stack expansion with notable cycling stability over 270 cycles (~27 days) is attained. The cost benefit evidenced by technoeconomic analysis together with the stability even under open-air conditions indicates the practical value of the present molecular system in grid-scale energy storage.
研究领域:
能源化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
SURFACE & COATINGS TECHNOLOGY
·
2024
·
IF 5.3
Ruiqing Hou,Youqing Li,Pingli Jiang,Shijie Zhu,Liguo Wang,Shaokang Guan
A controllable corrosion rate is an ideal condition for magnesium (Mg) alloy as biodegradable metallic materials. Calcium carbonate (CaCO 3 ) coating has been proven to possess a robust anti-corrosion property for Mg alloy. To further regulate the morphology and corrosion protection ability of the CaCO 3 coating, in current study, different organic molecules, including amino acids (Tyr and Glu), amine (DOPA), proteins (COL and BSA) and peptide (CPP), were added into the coating formation electrolyte, affecting the morphology, polymorph composition, and the crystal size distribution of precipitated CaCO 3 . The results revealed that Tyr exhibited little effect on the polymorph composition of the CaCO 3 -based coating, while Glu, DOPA, COL and BSA generally promoted the formation of vaterite but inhibited the formation of rod-like aragonite precipitates and calcite in the coatings. In contrast, CPP suppressed the precipitation of CaCO 3 crystals because of its high affinity to Ca 2+ ions. The addition of those organics reduced the size of calcite crystals. Consequently, the organic molecules mediated CaCO 3 -based coatings showed better compactness and homogeneity, which maintained the strong adhesion strength of the coatings to the substrate and further enhanced the corrosion protection abilities of the coating for the substrate. The results of the study pave the way for the development of CaCO 3 -based coatings with advanced properties for Mg alloys as biomedical materials .
研究领域:
材料科学
·
生物医学工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Yizhan Wang,Yunhui Shi,Jiawei Qiu,JiaBao Cheng,Yao Xu,Yongxin Wang
The intercalation of organic molecules is a promising approach to modulate the structure of 2D transition metal borides (MBenes), aiming to enhance charge transport and improve electrochemical performance in energy storage applications. However, key questions remain regarding how organic molecules with diverse functionalities penetrate and align between the MBene layer, as well as the mechanism of charge redistribution during intercalation. Addressing these questions is crucial for guiding the design of Organic-MBene heterostructures. To this end, a comprehensive approach combining theoretical calculations and experimental analyses was employed to explore the self-assembly mechanisms of organic molecules featuring N, O, S and tertiary amine end groups on the MoB-MBene surface. Experimental characterizations confirm that the interaction between MoB and organic compounds depends on the end groups. First principles calculations demonstrate that organic molecules tend to adopt a flat configuration on the MoB surface during molecular assembly. Calculations also reveal that the binding and charge transfer processes from organic molecules to MoB are highly dependent on the specific end groups, consistent with experimental observations. Furthermore, the effect of combining organic molecules with MoB on battery performance was further discussed, offering new insights for advancing the research and development of MBenes in aqueous battery systems.
研究领域:
材料科学
·
物理化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nature Communications
·
2021
·Vol. 12
·期 1
·1-7
·
IF 14.919
Zhang Mingming,Zhao Lili,Xie Jiahao,Zhang Qian,Wang Xiaoyu,Yaqoob Najma,Yin Zhengmao,Kaghazchi Payam,Zhang San,Li Hua,Zhang Chunfeng,Wang Lei,Zhang Lijun,Xu Weigao,Xing Jun
Low-dimensional hybrid perovskites have demonstrated excellent performance as white-light emitters. The broadband white emission originates from self-trapped excitons (STEs). Since the mechanism of STEs formation in perovskites is still not clear, preparing new low-dimensional white perovskites relies mostly on screening lots of intercalated organic molecules rather than rational design. Here, we report an atom-substituting strategy to trigger STEs formation in layered perovskites. Halogen-substituted phenyl molecules are applied to synthesize perovskite crystals. The halogen-substituents will withdraw electrons from the branched chain (-R-NH 3 + ) of the phenyl molecule. This will result in positive charge accumulation on -R-NH 3 + , and thus stronger Coulomb force of bond (-R-NH 3 + )-(PbBr 4 2− ), which facilitates excitons self-trapping. Our designed white perovskites exhibit photoluminescence quantum yield of 32%, color-rendering index of near 90 and chromaticity coordinates close to standard white-light. Our joint experiment-theory study provides insights into the STEs formation in perovskites and will benefit tailoring white perovskites with boosting performance.
研究领域:
材料科学
·
光学工程
·
化学
✓ 已验证
DOI
高影响因子
Nano Energy
·
2021
·
IF 17.881
Gabriel Sikukuu Nambafu,Kumar Siddharth,Cheng Zhang,Tianshou Zhao,Qing Chen,Khalil Amine,Minhua Shao
Symmetric redox flow batteries utilizing a single redox active material as catholyte and anolyte, offer a plausible and unique strategy to alleviate cross-contamination issues during cycling, making them an ideal energy storage device for large scale applications. In this work, a low-cost riboflavin organic molecule is coupled with a 2,2,6,6-Tetramethylpiperidinyl-N-oxyl (TEMPO) radical molecule to form a single Riboflavin-TEMPO (RIBOTEMPO) bifunctional redox active material, which is used in both aqueous anolyte and catholyte. Cyclic voltammetry analysis of the combined molecule displays electrochemically reversible reactions for the redox couples at −0.72 V and 0.51 V versus Hg/Hg 2 SO 4 , leading to a theoretical cell voltage of 1.23 V. A symmetric cell testing demonstrated over 100 consecutive charge/discharge cycles with nearly 80% coulombic efficiency and capacity retention of 44.7% at a current density of 2.5 mA cm −2 . By utilizing a pH neutral supporting electrolyte , a low-cost, safe, and environmental-friendly redox flow battery is achieved. This work provides a pathway for the design and development of bifunctional redox active molecules for symmetric battery applications.
研究领域:
化学
·
能源科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
SOLAR ENERGY MATERIALS AND SOLAR CELLS
·
2023
·
IF 6.9
Chunying Ma,Chu Zhang,Shennan Chen,Yongchun Ye,Lei Sun,Liguo Gao,Yusran Sulaiman,Tingli Ma,Miaogen Chen
Perovskite solar cells (PSCs) have attracted a lot of attention from researchers as the most promising photovoltaic devices due to their outstanding power conversion efficiency (PCE) and low-cost. Although the PSC have reached a PCE over 25%, the interface between the perovskite and hole transport layer (HTL) still is a crucial factor limiting higher PCE and long-term stability. In this work, we choose an organic molecule Bis(trifluoromethyl)benzo amide (BTFZA) to passivate defects at the perovskite/HTL interface. Owing to a strong interaction with uncoordinated Pb 2+ , the BTFZA effectively passivated the surface defects , remarkably promoted carrier transportation. As a result, the perovskite device based on BTFZA surface modification showed a PCE increase of 16.4% over the control device. Especially, the fill factor (FF) and the open-circuit voltage (V OC ) of the modified device increased significantly. In addition, the unencapsulated BTFZA-modified device maintains better PCE compared to the control device after aging for over 600 h in ambient air with extreme humidity and temperature conditions. Results suggested that the introduction of BTFZA is an effective way to regulate the surface of perovskite film aiming at highly efficient and stable perovskite solar cells.
研究领域:
材料科学
·
光伏技术
✓ 已验证
DOI
高影响因子
Nanoscale
·
2025
·
IF 5.1
Cai-Xia Zheng,Ai-Jun Jiao,zhenhai fu,Yu-Xia Hu,Min-Peng Li,Hong-Yan Li,Wei-Hai Yi,Xiao-Rui Wang,Meng-Chao Liu,Fuliang Zhu,Mao-Cheng Liu
MXenes are promising 2D-layered anode materials for rechargeable batteries due to their outstanding electrical conductivity, high specific surface area, and tunable surface functional groups. However, serious self-stacking of the layered structure and the sluggish sodium diffusion kinetics lead to inferior rate capability and cycling stability. Herein, an organic molecular pillaring strategy is reported to enlarge the interlayer spacing of Ti3C2 through a dehydration condensation reaction between the •COOH groups in 3,3',4,4'-benzene tetracarboxylic acid (BTCA) molecules and the•NH2 groups of Ti3C2-NH2, which enables rigid organic BTCA molecules to be chemically pillared into the interlayers of Ti3C2 (Ti3C2-BTCA). The rigid organic BTCA molecules not only play a dual role of pillar and strain effects in Ti3C2 layers, but also expand the interlayer spacing. Therefore, they can significantly enhance the rate capability and cycling stability of Ti3C2. The Ti3C2-BTCA exhibits a reversible capacity of 182.30 mAh g-1 at a current density of 0.1 A g-1 after 2000 cycles, and maintained a reversible capacity of 77.9 %. Moreover, the sodium diffusion coefficients of Ti3C2-BTCA are 6.6×10-7 cm2 s-1. Ti3C2-BTCA shows a relatively low sodium diffusion barrier and a high sodium diffusion coefficient compared with Ti3C2. The interlayer engineering based on the organic molecular pillaring strategy is significant and meaningful for expanding the interlayer spacing of Ti3C2. This work provides theoretical guidance and new perspectives for the development of Na+ storage materials with high-rate capability.
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
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Kun Liu,Junping Niu,Yijia Bai,Jianlei Qi,Limin Han,Ning Zhu,Ligang Yan
Ligand engineering has proven to be an effective strategy for tuning and controlling the microenvironment of coordinated metal centers, highlighting the critical bridge between the activity and structural features of catalysts during electrocatalytic CO 2 reduction reactions (eCO 2 RR). However, the limited availability of diverse organic ligands has hindered the development of novel high-performing electrocatalysts. In contrast, small organic molecules have been widely used in the fabrication of metal complexes due to their well-defined functionalities, low cost, and easy accessibility. Herein, functionalized small organic molecules were employed to prepare a new type of Bi-based heterogeneous molecular catalyst. These molecular catalysts enhance both electrical conductivity and catalytic activity for converting CO 2 to formate in the eCO 2 RR. The relationship between the structure and electrochemical performance of organic-functionalized Bi-based heterogeneous catalysts was thoroughly investigated. Comprehensive characterization and kinetic studies demonstrated that the functional groups of the organic molecules construct bond pathways for electron transfer and promote the transformation of the active phase from Bi to Bi 2 O 2 CO 3 . In-situ Raman spectroscopy reveal that the organic molecules remain intact during the structural reorganization, which is beneficial for the sustained generation of Bi 2 O 2 CO 3 active site during the eCO 2 RR process. Consequently, the organic functionalized Bi-based catalysts achieved a high formate Faradaic efficiency (FE HCOO - ) of 89.8 % and a high current density (j HCOO - ) of 40.0 mA cm −2 at a potential of −0.95 V vs. RHE in an H-type cell. This work establishes a novel strategy for creating active heterogeneous catalysts using small organic molecules, opening new avenues for the development of efficient electrocatalysts for CO 2 reduction.
研究领域:
化学
·
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF PETROLEUM SCIENCE AND ENGINEERING
·
2020
·
IF 3.706
Rukuan Chai,Yuetian Liu,Qianjun Liu,Wenhuan Gu
The mechanism of calcite-organic molecule-water interaction mechanism in oil-wet formation and alteration of carbonates is still ambiguous. This paper combines atomic force microscope (AFM), X-ray photoelectron spectroscopy (XPS) and molecular dynamic (MD) simulation to investigate the regularity and mechanism of calcite-organic molecule-water interaction at the molecular scale. First, the calcite-organic molecule-water interaction regularities, i.e., wettability alteration process, were studied using AFM, XPS and MD. AFM, XPS and MD results all demonstrated that acetic acid adsorbs stably on the calcite surface and can-not be displaced by water molecules, while the resistance to water displacement of the other three organic molecules decreased with decreasing molecular polarity. Subsequently, MD was used to analyze the calcite-organic molecule-water interaction mechanism from three perspectives, including the organic molecule-calcite interaction, the organic molecule-organic/water molecule interaction, and the effect of polar molecules. In the organic molecule-calcite interaction, the adsorption intensity of organic molecules on calcite surface decreases as their molecular polarity decreases. Stronger molecular polarity results in tighter adsorption layer and lower adsorption energy. In the organic molecule-organic/water molecule interaction, the interaction intensity increases as the polarity difference between the two molecules decreases. Larger polarity difference causes stronger miscibility and lower interaction energy. For polar molecules effect, the presence of polar molecules stabilizes the non-polar molecules adsorption and diminishes the displacement efficiency of water molecules. Consequently, this paper proposes the bulk adsorption mechanism to reasonably explain the wettability formation and alteration mechanism of calcite surface, which is of great importance for targeted enhanced oil recovery studies.
研究领域:
地质学
·
化学
·
分子生物学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）