Journal of Environmental Sciences
·
2021
·
IF 5.565
Ji Li,Chenlu Shi,Wenbin Zeng,Yaru Wang,Zebin Hong,Yibing Ma,Liping Fang
Electron shuttles such cysteine play an important role in Fe cycle and its availability in soils, while the roles of pH and organic ligands in this process are poorly understood. Herein, the reductive dissolution process of goethite by cysteine were explored in the presence of organic ligands. Our results showed that cysteine exhibited a strong reactivity towards goethite – a typical iron minerals in paddy soils with a rate constant ranging from 0.01 to 0.1 hr −1 . However, a large portion of Fe(II) appeared to be “structural species” retained on the surface. The decline of pH was favorable to generate more Fe(II) ions and enhancing tendency of Fe(II) release to solution. The decline of generation of Fe(II) by increasing pH was likely to be caused by a lower redox potential and the nature of cysteine pH-dependent adsorption towards goethite. Interestingly, the co-existence of oxalate and citrate ligands also enhanced the rate constant of Fe(II) release from 0.09 to 0.15 hr −1 ; nevertheless, they negligibly affected the overall generation of Fe(II) in opposition to the pH effect. Further spectroscopic evidence demonstrated that two molecules of cysteine could form disulfide bonds (S-S) to generate cystine through oxidative dehydration, and subsequently, inducing electron transfer from cysteine to the structural Fe(III) on goethite; meanwhile, those organic ligands act as Fe(II) “strippers”. The findings of this work provide new insights into the understanding of the different roles of pH and organic ligands on the generation and release of Fe induced by electron shuttles in soils.
研究领域:
土壤科学
·
环境化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Yufan Yuan,Fangling Guan,Chenglong Yu,Danping Li,Faying Lai,Huajun Huang,Jinbao He,Yanpeng Gao,Hansun Fang
Soil is an important sink for various pollutants. Recent findings suggest that soil and sediment would spontaneously form HO • through Fenton or Fenton-like reactions under natural conditions. In this study, the effects and mechanisms of organic ligands (OLs) on the occurrence of HO • in surface soil/sediment were experimentally and computationally examined. Results confirmed that HO • generation was ND-12.92 nmol/g in surface soil/sediment, and the addition of EDTA-2Na would significantly enhance the yields of HO • by 1.4–352 times. Moisture was the decisive factor of soil HO • generation. The release of Fe(II) from solid into the aqueous phase was essential for the stimulation of HO • in EDTA-2Na suspensions. Furthermore, complexation reactions between Fe(II) and OLs would enhance single electron transfer (SET) reactions and the formation of O 2 •- . Interestingly, for specific OLs, their stimulations on SET and formation of O 2 •- would depress HO • generation. Provoking HO • generation by OLs could be efficiently used to degrade sulfamethoxazole in rice field sediment. The study provided new knowledge on how commonly synthetic OLs affect the HO • generation in surface soil/sediment, and it additionally shed light on the engineered stimulation of in-situ Fenton reactions in natural soil/sediment.
研究领域:
环境科学
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化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
MATERIALS CHEMISTRY AND PHYSICS
·
2019
·
IF 2.781
Lei Huang,Zhihui Yang,Yujun Shen,Peng Wang,Baocheng Song,Yingjie He,Weichun Yang,Haiying Wang,Zhenxing Wang,Yongsheng Chen
Coordination bonds of ligands and metal ions are generally considered for improving agglomeration during the synthesis of metal oxides . However, the strong interactions always limit the performance due to the requirement of additional energy and calcination . A new strategy of synthesizing ZnO particles is proposed through a hydrothermal inducing redox method by using 2-methyl imidazole and Zn(NO 3 ) 2 . In situ direct redox between this organic ligand and NO 3 − in a hydrothermal condition is confirmed radical change instead of the simple coordination between organic ligands with Zn 2+ in traditional method. The directly acquired ZnO particles possessing uniform dumbbell-like morphology have no obvious agglomeration. The yield reaches >95%. In particular, the synthesis mechanism and morphology evolution during the ZnO aggregates growth were carefully explored and proposed. Density functional theory (DFT) and surface energy calculations demonstrated the effects of activity variation of reactive groups and preferred growth surface of ZnO crystals. This work gives new insights into new synthesis strategy of ZnO particles via hydrothermal condition.
研究领域:
材料科学
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化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF THE AMERICAN CERAMIC SOCIETY
·
2014
·Vol. 97
·期 6
·1931-1936
·
IF 2.428
Yunjuan He,Nan Chen,Guoping Du
LaOF:Eu 3+ nanoparticles were successfully prepared by annealing LaF 3 :Eu 3+ nanocrytsals which were capped with SiO 2 shell. The SiO 2 shell effectively prohibited the growth of LaF 3 :Eu 3+ nanocrystals during the annealing process, and it was etched off after annealing to obtain the LaOF:Eu 3+ nanoparticles. The LaOF:Eu 3+ nanoparticles had a size comparable to the original LaF 3 :Eu 3+ nanoparticles. Inorganic–organic hybrid nanoparticles of LaF 3 :Eu 3+ and LaOF:Eu 3+ nanoparticles with thenoyltrifluoroacetone (TTA) ligands were prepared. Strong luminescence as a result of the energy transfer from the TTA organic ligands to the LaF 3 :Eu 3+ and LaOF:Eu 3+ nanoparticles was observed. The LaOF:Eu 3+ -based hybrid nanoparticles exhibited stronger luminescence intensity and broader excitation spectral range than the LaF 3 :Eu 3+ -based hybrid nanoparticles. Effect of the content of TTA ligands on the luminescence of the LaOF:Eu 3+ nanoparticles was investigated in detail.
研究领域:
材料科学
·
光学
✓ 已验证
DOI
高影响因子
CRYSTENGCOMM
·
2015
·Vol. 17
·期 29
·5569-5578
·
IF 4.034
Ai-Xiang Tian,Ya-Li Ning,Jun Ying,Guo-Cheng Liu,Xue Hou,Tian-Jiao Li,Xiu-Li Wang
By using two kinds of organic ligands (1-benzyl-1H-(1,2,4)triazole (2-btz) and 1-benzyl-1H-(1,3,4)triazole (3-btz)), six polyoxometalate (POM)-based compounds were hydrothermally synthesized and structurally characterized, [Ag4(2-btz)4(HPMo2VMo10VIO40)] (1), [Ag4(2-btz)4(SiW12O40)] (2), [Ag4(2-btz)5K(SiWVW11VIO40)]·13H2O (3), [Cu4(2-btz)16(Mo8O26)2] (4), [Cu3(3-btz)8(H2O)4](PMo12O40)2·4H2O (5) and [Cu7(3-btz)16(OH)2(H2O)4(P2W18O62)2]·16H2O (6). Compounds 1 and 2 are isostructural with two sets of Ag–(2-btz) chains linked by Keggin anions to construct a “ladder”. Adjacent “ladders” are further connected by Ag1–O13 bonds to build a 3D framework. In compound 3, the anion dimers are linked by Ag5–O9 bonds to form a 1D chain. The chains are fused by Ag3 and K ions and a 3D framework of 3 is built. In compound 4, the Mo8 anions are linked by [Cu(2-btz)4]2+ subunits to construct a 3D structure. By changing 2-btz to 3-btz, we obtained a linear tri-nuclear cluster [Cu3(3-btz)8(H2O)4]6+ in compound 5. The discrete PMo12 anions combine with tri-nuclear clusters through hydrogen bonding interactions to construct a 2D supramolecular layer. Compound 6 contains a cycle tri-nuclear cluster-supporting anion [Cu3(3-btz)6(OH)(H2O)2(P2W18O62)]−, which is further connected by one [Cu(3-btz)4]2+ subunit to construct a discrete anion dimer. The title compounds show good electrocatalytic activities for reducing nitrite, hydrogen peroxide and bromate. These compounds also exhibit excellent photocatalytic activities for the degradation of methylene blue (MB, 1–6 as catalysts) and Rhodamine B (RhB, 5 and 6 as catalysts). Additionally, the magnetic properties of compounds 5 and 6 have been investigated.
研究领域:
无机化学
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材料科学
✓ 已验证
DOI
高影响因子
APPLIED ORGANOMETALLIC CHEMISTRY
·
2025
·Vol. 39
·期 5
·e70103
·
IF 0
Palanisamy Vasudhevan,Dong Yu,Ruoyu Zhang,Mysoon M. Al-Ansari,Velu Manikandan,Hui Ma,Saurav Dixit,Shengyan Pu
Chlorinated aromatic chemicals are highly hazardous, transmissible, and bioaccumulative. Developing an economically feasible catalytic method to facilitate the effective removal of chlorinated aromatic pollutants is critical for contamination prevention. The current study extensively investigated the utilization of organic ligands such as citrate (CA) and ethylenediaminetetraacetic acid (EDTA) to increase Fe(II)-activated persulfate (PS) for 4-chlorophenol (4-CP) and 3-chlorobenzoic acid (3-CB) degradation in water. The decomposition and consumption ability of persulfate in PS alone and Fe(II)/PS systems for 4-CP and 3-CB was very low because of the rapid utilization as well as discontinuous availability of Fe(II), which indicates the decline of Fe(III) to Fe(II). But, when using the citrate/Fe(II)/PS and EDTA/Fe(II)/PS combinations, the degradation of 4-CP and 3-CB was 78.86%, 75.01% and 84.84%, 80.99% within 30 min, respectively. The significant enhancement is due to both ligand-to-metal transfer of charges process, and this increased the process of rate determination through carrying electrons into the citrate and EDTA ligands to Fe(III), generating Fe(II). In addition, the 4-CP and 3-CB degradation facilitated with citrate/Fe(II)/PS and EDTA/Fe(II)/PS systems was efficiently degraded at acidic pH (2.0–6.0) conditions. The pseudo-first-order kinetics model accurately predicted 4-CP and 3-CB degradation in the organic ligand/Fe(II)/PS systems. The degradation percentage of 4-CP and 3-CB increased with increasing PS and Fe(II) concentrations. Moreover, both sulfate and hydroxyl radicals formed by citrate/Fe(II)/PS and EDTA/Fe(II)/PS systems were identified as major reactive oxygen species for 4-CP and 3-CB decomposition. The present investigation recommends an alternate strategy to enhance the Fe(II)-activated persulfate mechanisms.
研究领域:
环境科学
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化学
✓ 已验证
产品关联
DOI
INORGANIC CHEMISTRY
·
2024
·
IF 4.3
Guanlei Gao,Si-Yu Xu,Xinghui Qi,Jie-Ru Yang,Peiqi Lin,Jin Chen,Xiao-Ying Huang,Ke-Zhao Du
The strategy of organic ligand exchange is proposed to tune the optical properties of organic–inorganic hybrid cuprous halides. In this work, the chiral ligand (S)-(−)-2,2′-bis(di-p-tolylphosphino)-1,1′-binaphthyl ((S)-Tol-BINAP) and achiral triphenylphosphine (PPh3) are introduced into cuprous halides CuX-PPh3-[(S)-Tol-BINAP] (X = Cl, Br, I) through organic ligand exchange. As a result, the mixed organic ligands can enhance second harmonic generation (SHG) and aggregation-induced emission (AIE) optical properties. Moreover, the title compounds exhibit progressively enlarged SHG effects along with heavier halogen substitution due to their stronger polarizability. In the meantime, the reduced π–π stacking interaction of the organic ligand will improve their photoluminescence quantum yield. The experimental results combined with the theoretical calculation clarify the structure–property relationship well. Furthermore, the title compounds have been developed for the application of latent fingerprint detection.
研究领域:
材料科学
·
化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nanoscale Research Letters
·
2014
·Vol. 9
·期 1
·1-7
·
IF 2.481
Ji Jianwei,Wang Guan,You Xiaozeng,Xu Xiangxing
Silicon quantum dots (Si QDs) attract increasing interest nowadays due to their excellent optical and electronic properties. However, only a few optoelectronic organic molecules were reported as ligands of colloidal Si QDs. In this report, N -vinylcarbazole - a material widely used in the optoelectronics industry - was used for the modification of Si QDs as ligands. This hybrid nanomaterial exhibits different spectroscopic properties from either free ligands or Si QDs alone. Possible mechanisms were discussed. This type of new functional Si QDs may find application potentials in bioimaging, photovoltaic, or optoelectronic devices.
研究领域:
材料科学
·
光学
·
生物医学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Yalan Zhang,Tinghuan Yang,Raja sekhar Bobba,Abiral Baniya,Tianqi Niu,Sally Mabrouk,Shengzhong Liu,Quinn Qiao,Kui Zhao
The combination of organic ligands and inorganic Pb–I frameworks in layered perovskites has bestowed upon them high structural tunability and stability, while their microscopic degradation mechanism remains unclear. Here, we found the key role of ligands in intrinsic structural stability and the consequent morphological evolution in layered perovskites during long-term ambient aging based on (GA)(MA)nPbnI3n+1 (GA = guanidinium, = 4) and (BDA)(MA)n−1PbnI3n+1 (BDA = 1,4-butanediammonium, < n > = 4) perovskites. The BDA-based perovskites have a low intrinsic stability due to high crystal formation energy (ΔH), which are prone to hydration during ambient aging. We overserved changed crystal orientation from perpendicular to parallel, a delayed charge populating time from <1 ps to >50 ps, an inhibited carrier transfer kinetics between quantum wells, an increase of 0.9 μs of charge carrier transport time and a decrease of 1.2 μs of charge carrier lifetime in the BDA-based film during ambient aging, which accounts for a large power-conversion efficiency (PCE) loss (14.2% vs 11.2%). By contrast, the GA ligand increases the intrinsic structural stability of perovskites, which not only yields an initial PCE as high as 20.0% but also helps retain excellent optoelectronic properties during aging. Therefore, only a slight PCE loss (20.0% vs 19.1%) was observed. Our work reveals the key role of organic–inorganic interaction affecting the intrinsic structural stability and optoelectronic properties, and provides a theoretical basis for the future design of stable and efficient optoelectronic devices.
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
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2022
·
IF 11.357
Meiqi Li,Na Chen,Huan Shang,Cancan Ling,Kai Wei,Shengxi Zhao,Biao Zhou,Falong Jia,Zhihui Ai,Lizhi Zhang
Heavy metals chelated with coexisting organic ligands in wastewater impose severe risks to public health and the ambient ecosystem but are also valuable metal resources. For sustainable development goals, the treatment of heavy metal complexes wastewater requires simultaneous metal–organic bond destruction and metal resource recovery. In this study, we demonstrated that a neutral pH electro-Fenton (EF) system, which was composed of an iron anode, carbon cloth cathode, and sodium tetrapolyphosphate electrolyte (Na6TPP), could induce a successive single-electron activation pathway of molecular oxygen due to the formation of Fe(II)-TPP complexes. The boosted •OH generation in the Na6TPP-EF process could decomplex 99.9% of copper ethylene diamine tetraacetate within 8 h; meanwhile, the released Cu ions were in situ deposited on the carbon cloth cathode in the form of Cu nanoparticles with a high energy efficiency of 2.45 g kWh–1. Impressively, the recovered Cu nanoparticles were of purity over 95.0%. More importantly, this neutral EF strategy could realize the simultaneous removal of Cu, Ni, and Cr complexes from real electroplating effluents. This study provides a promising neutral EF system for simultaneous heavy metal complexes wastewater treatment and resource recovery and sheds light on the importance of molecular oxygen activation in the field of pollutant control.
研究领域:
环境科学
·
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Science Bulletin
·
2019
·
IF 6.277
Yang An,Yuanyuan Liu,Hongtao Bian,Zeyan Wang,Peng Wang,Zhaoke Zheng,Ying Dai,Myung-Hwan Whangbo,Baibiao Huang
UiO-67 is a Zr-based metal–organic framework (MOF) containing an organic linker namely, the dianion of biphenyl-4,4′-dicarboxylic acid (bpdc). Ce 4+ metal ions (0.02 Ce to Zr atom ratio) were incorporated into UiO-67 via partially replacing bpdc with the dianion of 2,2′-bipyridine-5,5′-dicarboxylic acid (bpydc); thus, the latter forms a bpydc-Ce complex. The resulting product (i.e., UiO-67-Ce) demonstrated a photocatalytic hydrogen evolution rate that was over 10 times higher than that of UiO-67. Through this modification, a new energy transfer channel is opened up. The energy transfer between the bpdc and bpydc-Ce ligands (i.e., from excited bpdc to bpydc-Ce) weakened the recombination of the charge carriers, which was confirmed by photoluminescence, emission lifetime, and transient absorption measurements. This study presents a new way to construct highly efficient MOF photocatalysts.
研究领域:
材料科学
·
化学
✓ 已验证
DOI
PubMed
高影响因子
NANOTECHNOLOGY
·
2022
·Vol. 33
·期 35
·355701
·
IF 3.953
Guoying Yao,Liang Zhao,Tao Zeng,Zhenyu Yang
Reduced-dimensional (RD) perovskites have shown attractive chemical and physical properties for optoelectronic applications. Incorporating large organic ligands enables infinite tunability in the components and structures. Theoretically, it is feasible to apply multiple types of organic ligands in a single RD crystal to achieve multiple-dimensional perovskites. However, the coexistence of different organic ligands commonly introduces competing crystal growths that inhibit the formation of a more complex crystal structure. Herein, we report a case of mixed-dimensional (MD) perovskite single crystal containing two types of sulfide-containing ligands. We show that the application of ketones can partially oxidize organothiol ligands in the precursor solution. The resultant disulfide-based ligands can be co-incorporated with the thiol-based ligand in a single MD perovskite crystal. X-ray diffraction confirmed that the structure contains both layered and isolated inorganic components constructed by face-sharing lead halide octahedra. Unlike conventional RD structures, the MD perovskite shows an enlarged bandgap with valence band maximum and conduction band minimum being spatially separated, and isotropic optical features, as revealed by x-ray diffraction, spectroscopies, and density functional theory computation.
研究领域:
材料科学
·
化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）