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CHEMICAL ENGINEERING JOURNAL · 2019 · IF 8.355

Cycle of Ni(II)-Ni(III)-Ni(II) in Ni-doped layered double hydroxides for activation of intercalated peroxydisulfate

Xin Huang,Xujie Zhou,Shaohong Han,Jizhi Zhou,Guangren Qian,Naiyun Gao

Peroxydisulfate (PDS) activation has attracted much attention for the treatment of drinking water systems. In this work, Ni-doped MgAl layered double hydroxides (Ni-LDHs, Ni:Mg = 1:100 to 1:1, molar ratio) were prepared for the activation of PDS via intercalation. Compared with the case without Ni, doping with Ni resulted in much higher phenol degradation at the same PDS dosage. This was attributed to the activation of PDS, as the PDS consumption increased with increasing Ni doping amount. Moreover, radicals corresponding to organic decomposition were detected in the presence of Ni. Physical characterization results reveal that Ni(II) was converted to Ni(III) with PDS and then reduced back to Ni(II) during organic decomposition. To our best knowledge, this is the first study to report a cycle of Ni(II)-Ni(III)-Ni(II) in LDHs for the efficient activation of PDS. This effect was also observed in cases of odorous substances such as 4-bromophenol, 2-methylisoborneol, and geosmin. Our work provides a promising approach for the activation of PDS by Ni-LDHs.

CAS / MDL: 2259-96-3
研究领域: 环境科学 · 化学
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Rationally engineered core-shell structured Fe0@FeS towards the efficacious synergistic Cr(VI) and Ni(II) removal

Zishen Lin,Chunli Zheng,Zhenxing Wang,Yuanzhe Peng,Guoqing Geng,Aibin Zhu,Chi He

As one category of promising and efficacious purification material toward environmentally harmful heavy metals, sulfidated amorphous zero-valent Iron (S@AZVI) exhibits unparalleled removal performance. Due to the disruptive crystal growth however, the irreversible loss of Fe 0 component during conventional synthesis route poses a substantial hindrance to its industrial application. To address this, we propose a post-sulfidation strategy to hinder the transformation of Fe 0 by altering the shell composition of AZVI from Fe 2 O 3 to FeS, which maintains a remarkable Fe 0 content up to 75.7 % over finally obtained S@AZVI, far higher than the material obtained through the one-step sulfidation . Attributing to the synergy of FeS shell and substantial Fe 0 , S@AZVI demonstrates impressive performance as the lowest free corrosion potential (−1.050 V) and work function (4.058 eV), and subsequently exhibits a notable enhancement in the removal efficiency of Cr(VI) and Ni(II), surpassing AZVI by 1.8 and 2.0 times, respectively. Results reveal that the adsorption, reduction, and coprecipitation constitute the mechanisms governing the removal of Cr(VI) and Ni(II). In practical electroplating wastewater experiments, S@AZVI effectively removes Cr(VI) and Ni(II) within a 60-min timeframe, meeting established emission standards. These findings provide valuable insights for future AZVI material synthesis for heavy metal elimination.

研究领域: 环境科学 · 材料科学
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2021 · IF 4.539

Superior adsorptive removal of azo dyes from aqueous solution by a Ni(II)-doped metal–organic framework

Xiu-Ling Li,Wei Zhang,Yong-Qing Huang,Qiang Wang,Ji-Min Yang

Toxic azo dyes pose a significant threat to all living organisms when they are directly discharged into aqueous environments. Therefore, new adsorbents with excellent adsorptive efficiencies are urgently required for the removal of azo dyes. Herein, the adsorption space, surface charge, morphological and structural defects, and mesostructure of MIL-101(Cr) were adjusted by Ni(II) doping to understand the effects of these factors on the adsorptive removal of anionic azo dyes such as Congo red (CR), methyl orange (MO), and acid chrome blue K (AC) from aqueous solution. The adsorption uptakes of Ni(II)-doped MIL-101(Cr) toward CR (1607.4 mg g −1 ) and MO (651.2 mg g −1 ) exceeded those of undoped MIL-101(Cr) by 31.4% and 23.4%, respectively, whereas Ni(II) doping decreased the adsorption uptake toward AC (161.0 mg g −1 ) by 50.2%. Ni(II) doping produced morphological and structural defects, resulting in a new mesoporous structure, which played a more prominent role than electrostatic interactions and adsorption space in increasing the adsorption uptake toward linear anionic azo dyes, such as CR and MO. Despite these effects, for nonlinear azo dyes such as AC the adsorption uptake was decreased by steric hindrance between the Ni(II)-doped MIL-101(Cr) adsorbent and the dye. Thus, the adsorption performance of Ni(II)-doped MIL-101(Cr) was found to be controlled by the synergetic interplay among electrostatic interactions, π–π interactions, steric hindrance, and the morphological and structural defects, pore volume , and mesoporous structure of the adsorbent.

研究领域: 环境科学 · 材料科学
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SEPARATION SCIENCE AND TECHNOLOGY · 2023 · IF 2.8

Comparative investigation on Ni(II) removal from electroplating wastewater by mineral adsorbent (CSAM) and ion-exchange resins

Mingjian Wang,Meiqing Zeng,Pingsan Wang,Yaochi Liu

The efficiency of Ni(II) removal from electroplating wastewater is highly correlated with different adsorption materials. A Ca-Si activated mineral adsorbent (CSAM) and two ion-exchange resins (732 and D152) were compared. The adsorption of Ni (II) by three materials is spontaneous and endothermic, and their adsorption capacities are similar (48.66–65.36 mg/g at 318K), but the dosage of CSAM is less (1.0 g/L for 50 mg/L Ni(II)), its adsorption is faster (<5 min) and pH range is wider (2–7). 10% NaCl, 1 mol/L HCl and 10% NaCl +1 mol/L HCl were used as desorbent agents, and CSAM exhibited an extremely low desorption rate (1.49–3.41%). The smaller separation factor (close to 0) and XPS analysis showed that the Ni(II) adsorption on CSAM was an irreversible chemical process, which was different from the three-stage adsorption of resins. The treatment of two kinds of electroplating wastewater with high and low concentration showed that CSAM not only had a higher Ni(II) removal rates (>98.4%), but also could efficiently remove Cu(II) (>98%), total-chromium (>79%) and COD (>66%). The treatment of Ni(II) containing electroplating wastewater with ion-exchange resins is greatly affected by the complexing agent. CSAM is more suitable for the treatment of electroplating wastewater containing various metals and organic matters.

研究领域: 环境科学 · 化学工程
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Journal of Physical Chemistry C · 2022 · IF 4.177

Ni(II) Tetra(4-carboxylphenyl)porphyrin-Sensitized TiO2 Nanotube Array Composite for Efficient Photocatalytic Reduction of CO2

Tongxin Xiao,Ying Chen,Yuning Liang

The photocatalytic conversion of CO2 into hydrocarbon fuels by utilizing abundant solar energy is a promising and eco-friendly approach to address the energy crisis and global warming. In this work, the sensitizer Ni(II) tetra(4-carboxylphenyl)porphyrin (NiTCPP) was successfully combined with TiO2 nanotube arrays (TiO2NTs) by three methods, and their performances in the photocatalytic reduction of CO2 under simulated solar irradiation were studied. The results showed that NiTCPP/TiO2NTs exhibit a greatly ameliorated photocatalytic activity, and the photocatalytic reduction activities of NiTCPP/TiO2NTs prepared by different methods were different. The catalyst prepared by the impregnation method displayed the highest photoreduction efficiency. The reduction rate of CO2 into CH4 was up to 33.89 μmol/cm2/h with a quantum efficiency of 0.65% (at 420 nm), about 5 times that of the bare TiO2NTs. The introduction of NiTCPP not only efficiently expands the light absorption range but also enhances the charge separation efficiency. Furthermore, a possible mechanism of its CO2 photoreduction performances was systematically presented.

研究领域: 材料科学 · 环境科学
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JOURNAL OF MOLECULAR STRUCTURE · 2022 · IF 3.841

A spectroscopic approach to identifying the out-of-plane conformations of Ni(II) meso-tetraphenylporphyrin in solution

Shenhao Wang,Qing Huang

Ni(II) meso-tetraphenylporphyrin (NiTPP) is a model molecule whose substituent causes out-of-plane (oop) deformations of the porphyrin macrocycle. Although the conformers of NiTPP in the solution had been tentatively explored, the determination of its specific conformers was controversial. In this work, based on the conformational search through molecular dynamics (MD), three energy lowest-lying conformers of NiTPP were sorted out, namely, the S 4 (staggered) conformer, the C 2 (eclipsed) conformer, and the C 1 (eclipsed-staggered) conformer. According to the high-precision free energy calculation based on density functional theory (DFT), the Raman and 1 H-NMR spectra of the three conformers were calculated. The actual spectra of NiTPP in solution resulted from the sum spectra of the mixture conformers, so with the consideration of the corresponding conformation weights, the experimental spectra could be stimulated. Our results showed that only at the low-frequency ∼215 cm −1 , did the Raman spectrum in solution differ significantly from that in solid powder. On the other hand, the 1 H-NMR spectra of the NiTPP conformers were remarkably different, and none of the single conformer's 1 H-NMR range could match the experimental 1 H-NMR spectrum. However, with the consideration of the existence of three dominant conformations, the observed 1 H-NMR spectrum could be well simulated, confirming the rational mixture of the three dominant conformers existing in the aqueous solution. Therefore, this work has not only resolved the different conformers of NiTPP in solution, but also provided an effective approach to combining DFT, Raman, and 1 H-NMR analytical tools for identifying different oop conformations of metalloporphyrins in solution.

CAS / MDL: 75-09-2 24144-92-1
研究领域: 化学 · 光谱学 · 理论计算
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INORGANICA CHIMICA ACTA · 2023 · IF 2.8

Efficient alcohol electro-oxidation based on a 3D Ni(II)-MOF with centrosymmetric Ni6 cluster

Tian-Yu Zhang,Xue-Qian Wu,Heng-Yu Ruan,Yi Yuan,Le Wang,Ya-Pan Wu,Qing-Wen Han,Ruan Chi,Dong-Sheng Li

Designing economical and efficient anode catalysts is critical for the commercial use of direct alcohol fuel cells (DAFCs). In this work, a novel Ni(II)-based metal–organic framework (MOF), {[Ni 3 ( μ 3 -OH)(TMBTI)(1,4-bib)(H 3 O)} n (H 6 TMBTI = 2,4,6-trimethylbenzene-1,3,5-triylisophthalate, 1,4-bib = 1,4-bis(1-imidazoly)benzene) (CTGU-38, CTGU = China Three Gorges University), was successfully synthesized through solvothermal method. Structural analyses reveal that the CTGU-38 possesses a unique Ni 6 ( μ 3 -OH) 2 (COO) 12 cluster and 3D porous framework with a rare (6,16)-connected topology. Further electrochemical experiments demonstrate that the CTGU-38 exhibits good electrocatalytic oxidation performance towards various alcohol fuel molecules, including the methanol oxidation reaction (MOR), ethanol oxidation reaction (EOR), n -propanol oxidation reaction (NPOR), and isopropanol oxidation reaction (IPOR), with peak current densities ranging from 26.9 to 54.46 mA cm −2 in alkaline solution. These results indicate that the CTGU-38 appears to be a potential non-noble metal-based electrocatalyst for DAFCs, and this work provides new insights into the design of more efficient electrocatalysts at the atomic scale for energy conversion.

研究领域: 材料科学 · 电化学 · 能源转换
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Inorganic and Nano-Metal Chemistry · 2017 · IF 0

Synthesis, structure, and photocatalytic activity of a novel Ni (II) coordination polymer based on p-aminohippuric acid

Ziao Zong,Xiangmin Meng,Xin Li,Caifeng Bi,Yuhua Fan

A novel Ni(II) coordination polymer, {[Ni(C9H9N2O3)2(H2O)2]·H2O}n(1)(C9H11N2O3, p-Aminohippuric acid, PAH), has been synthesized and characterized by single-crystal X-ray diffraction, elemental analysis, IR spectra, and thermal analysis. Single-crystal X-ray analysis reveals that each Ni(II) ion is six-coordinated by two coordinated water molecules, two carboxylate oxygen atoms, and two nitrogen atoms from PAH forming a octahedral geometry. The complex features a 2-nodal 2,4-connected network with unprecedented Schläfli symbol of (42)(4)2. In addition, the photocatalytic studies indicate that this complex is a good candidate for the photocatalytic degradation of rhodamine B.

CAS / MDL: 61-78-9
研究领域: 材料化学 · 配位化学 · 环境科学
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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Single site Ni(II) anchored tetraethylene pentamine for enhancing CO2 kinetic adsorption rate and long-term cyclic stability

Shichao Zhang,Wenbin Chen,Junju Mu,Jianyu Han,Chaofeng Zhang,Zhuyan Gao,Jian Zhang,Yehong Wang,Feng Wang

Rapid kinetic adsorption and long-term cyclic stability are two of the major obstacles to the industrialization of solid amine adsorbents. The morphology and dispersibility of the organic amine in the pore structure of the support can strongly affect the adsorption rate and stability of CO 2 . In this work, we propose a strategy that enhances the dispersion and stability of tetraethylene pentamine (TEPA) via anchoring TEPA with single site Ni(II) in the pore of the commercial mesoporous silica gel (SG). The microscopic morphology and dynamic behavior of TEPA molecules in the adsorbents preparation process were explored by molecular dynamics simulation, which proved that the dispersibility of anchored TEPA in the porous structure has been improved, resulting in enhanced mass transfer and increased kinetic adsorption rate. The anchored Ni-TEPA/SG adsorbents exhibit a 37.5% faster kinetic adsorption rate than TEPA/SG adsorbents at 30 wt% TEPA loading, and the time required to reach 90% of maximum adsorption capacity is shortened by 6 times. Besides, the CO 2 adsorption performance of the optimized Ni-TEPA/SG adsorbent remains unchanged after 20 cycles, consolidating the potential of our proposed strategy in improving the kinetic adsorption rate and cyclic stability of solid amine adsorbents as well as promoting its industrialization.

CAS / MDL: 13478-00-7 112-57-2
研究领域: 材料科学 · 环境科学
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Journal of Environmental Chemical Engineering · 2023 · IF 7.7

An efficient method for separation of Ni(II) and Co(II) with novel extractant NNPA: Synthesis, characterization, extraction behaviors, crystal structures and DFT computational studies

Qiyuan Zheng,Zuoying Cao,Shengxi Wu,Qinggang Li,Mingyu Wang,Wenjuan Guan,Guiqing Zhang

As the production and consumption of lithium-ion batteries increase, high purity Ni(II) and Co(II) products are becoming increasingly critical as key raw materials for battery cathodes. However, the clean and efficient separation of Ni(II) and Co(II) has been a bottleneck problem since they often coexist in ores and secondary resources and have similar ionic radii, oxidation states, and coordination numbers. Thus, this paper proposes a novel extractant (NNPA) and a breakthrough method to separate Ni(II) and Co(II). The effects of chloride ion concentration , pH value, temperature, O/A ratio and extraction time on extractant selectivity and extraction efficiency were investigated. Under optimum conditions, NNPA demonstrated high extraction ability (E = 94.6 %) and selectivity (β Ni(II)/Co(II) = 481) for Ni(II) at pH 0, whereas at pH 6, it has high extraction ability (E = 93.9 %) and selectivity (β Co(II)/Ni(II) = 510.88) for Co(II). To provide in-depth insights into the Ni(II) and Co(II) separation mechanism, based on the single crystal XRD analyses of the extracted Ni(II) complex and the extracted Co(II) complex, DFT calculations were performed. The results show that the extraction order of NNPA is NNPANiHCl 3 > NNPACoCl 2 > NNPANiCl 2 (H 2 O) 2 . Due to the different selectivity of NNPA towards Ni(II) or Co(II) at different pH values, it is able to greatly reduce the consumption of extractant and significantly shorten the extraction process flow by selectively extracting the low concentration Ni(II) or Co(II) from Ni(II)-Co(II) solutions, thereby improving efficiency, reducing energy consumption and achieving cleaning production.

研究领域: 化学工程 · 材料科学 · 环境科学
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TEXTILE RESEARCH JOURNAL · 2022 · IF 2.455

Construction of a novel hydrogel composite with polylactic acid nonwoven fibers: rapid and effective removal of Pb(II) and Ni(II)

Zhi-Ke Wang,Ting-Ting Li,Hai-Tao Ren,Hao-Kai Peng,Bing-Chiuan Shiu,Jia-Horng Lin,Ching-Wen Lou

In this study, a hydrogel composite adsorbent structure was reported and showed satisfactory adsorption performance. The study uses polylactic acid melt-blown nonwoven fabric to optimize and improve the adsorption performance of the hydrogel. The results show that the nonwoven fabric structure enables the composite material to reach the swelling equilibrium faster than the hydrogel. The adsorption-isotherm model found that the adsorption capacity of composite materials Pb(II) and Ni(II) reached 416.07 and 243.10 mg/g, respectively, and still had high removal efficiency at low pH. The composite material has low cost and can be reused, which solves the problems of difficulty in recovery of the hydrogel adsorbent, low strength, and easy damage, and promotes the industrialization of the hydrogel as an adsorbent.

研究领域: 环境科学 · 材料科学
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RSC Advances · 2016 ·Vol. 6 ·期 25 ·20542-20550 · IF 3.289

Preparation of a nano-MnO2 surface-modified reduced graphene oxide/PVDF flat sheet membrane for adsorptive removal of aqueous Ni(II)

Renjie Li,Lifen Liu,Yuehua Zhang,Fenglin Yang

In this paper, nanoscale MnO2 particles were attached onto the surface of a PVDF flat sheet membrane, step by step, first through dispersion of graphene oxide (GO) in the PVDF membrane, then reduction of immobilized GO by hydroiodic acid and further micro-wave assisted oxidation of RGO (reduced graphene oxide) by KMnO4 and formation of MnO2 on GO. The SEM observation revealed an asymmetric structure with a finger-like transition layer dominating the membrane of PVDF/MnO2. The uniform distribution of MnO2 on the membrane is revealed by EDX and XPS analysis. The attached MnO2 endowed the membrane with high adsorption capacity for aqueous Ni(II). The adsorption was spontaneous and endothermic, fitting a pseudo-first-order kinetic model and Freundlich isotherm model well. The pure water flux and stable permeation flux of the PVDF/MnO2 membrane reached 31.2 L m−2 h−1 and 9.0 L m−2 h−1 under 0.1 MPa, which were 2.3 and 2.6 times those of the PVDF membrane. The analysis of the fouling resistance and flux recovery ratio indicated that the PVDF/MnO2 membrane had better antifouling properties than the PVDF membrane, attributed to the changes of membrane morphologies and surface hydrophilicity. The PVDF/MnO2 membrane had a high removal ratio (≥87.4%) of Ni2+ in dynamic adsorption. Meanwhile the Ni(II) adsorbed membrane could be easily regenerated by a 0.1 M HNO3 solution.

CAS / MDL: 13478-00-7
研究领域: 材料科学 · 环境工程
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