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ORGANIC ELECTRONICS · 2022 · IF 3.868

Amidine thiourea as a multifunctional modifier of buried interface for effective perovskite solar cells with reduced lead leakage

Meiling Yang,Rujia Hu,Jin Kang,Yaoming Xiao,Gaoyi Han,Wenjing Hou

The defects at buried SnO 2 /perovskite interface can influence the performances of perovskite solar cells by causing the poor perovskite crystallinity , bad interface connection, undesired interfacial recombination and electron transfer efficiency. Now, multifunctional amidine thiourea is used to modify the buried SnO 2 /perovskite interface. The amidine thiourea can passivate the interface defects by the electron donation roles of N and S atoms, improve the electron transfer efficiency by enhancing the interface connection and regulating the interface energy level matching, reduce lead leakage and reinforce the structural stability of device by the coordination and hydrogen bond interaction. The perovskite solar cells with the amidine thiourea modification exhibit an enhanced power conversion efficiency (20.48%) and stability, outperforming than that of control device (18.65%). Modifying the buried interface with small organic molecule is a feasible and efficient method to improve the performances of PSCs.

研究领域: 材料科学 · 能源技术 · 界面化学
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ACS Applied Materials & Interfaces · 2024 · IF 8.3

Efficient and Stable CuSCN-based Perovskite Solar Cells Achieved by Interfacial Engineering with Amidinothiourea

Ziqi Tang,Disheng Yao,Ying Li,Chao Li,Tian Xia,Nan Tian,Jilin Wang,Guoyuan Zheng,Shuyi Mo,Fei Long,Bing Zhou

Cuprous thiocyanate (CuSCN) emerges as a prime candidate among inorganic hole-transport materials, particularly suitable for the fabrication of perovskite solar cells. Nonetheless, there is an Ohmic contact degradation between the perovskite and CuSCN layers. This is induced by polar solvents and undesired purities, which reduce device efficiency and operational stability. In this work, we introduce amidinothiourea (ASU) as an intermediate layer between perovskites and CuSCN to overcome the above obstacles. The characterization results confirm that ASU-modified perovskites have eliminated trap-induced defects by strong chemical bonding between –NH– and C═S from ASU and under-coordinated ions in perovskites. The interfacial engineering based on the ASU also reduces the potential barrier between the perovskite and CuSCN layers. The ASU-treated perovskite solar cells (PSC) with a gold electrode obtains an improved power conversion efficiency (PCE) from 16.36 to 18.03%. Furthermore, after being stored for 1800 h in ambient air (relative humidity (RH) = 45%), the related device without encapsulation maintains over 90% of its initial efficiency. The further combination of ASU and carbon-tape electrodes demonstrates its potential to fabricate low-cost but stable carbon-based PSCs. This work finds a universal approach for the fabrication of efficient and stable PSCs with different device structures.

研究领域: 材料科学 · 可再生能源 · 光伏技术
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2024 · IF 4.9

Electrochemical and surface investigations of N, S codoped carbon dots as effective corrosion inhibitor for mild steel in acidic solution

Lei Guo,Lei Zhu,Savaş Kaya,Rui Sun,Alessandra Gilda Ritacca,Kai Wang,Jun Chang

Mild steel is a versatile, inexpensive, highly flexible, and easily weldable material widely used in construction, pipelines, transportation, shipping, and other industries. However, it is also extremely susceptible to corrosion processes under the influence of weather phenomena, posing a significant threat to society and human health. In this work, we investigated the corrosion inhibition capacity of a new type of N, S codoped carbon dots (N, S-CDs) on Q235 carbon steel in the acidic medium. The goal product was synthesized by hydrothermal method using o-phenylenediamine and amidinothiourea as precursors. Combined with electrochemistry, Fourier transform infrared (FTIR) spectroscopy, scanning electrochemical microscopy (SECM), and theoretical calculations, the inhibition properties of N, S-CDs on Q235 carbon steel in HCl solution were evaluated. The potentiodynamic polarization (PDP) curves and electrochemical impedance spectroscopy (EIS) results indicated that the corrosion inhibition efficiency reached 90.3 % and 92.4 % at 100 mg/L concentration, respectively. Indeed, the presence of N, S-CDs reduced the electric double-layer capacitance, increased the thickness of the adsorption film on the carbon steel surface, and reduced the corrosion current density, resulting in a delay of corrosion. X-ray photoelectron spectroscopy (XPS) analysis and surface characterization confirmed the successful doping of N, S and the formation of adsorption films, the Langmuir adsorption isotherm also confirmed the superior inhibition of N, S-CDs on the surface of Q235 carbon steel through physical and chemical adsorption mechanisms. At the same time, quantum chemical calculations and molecular dynamics (MD) simulations revealed its inhibition mechanism at the molecular/atomic level.

CAS / MDL: 2114-02-5
研究领域: 材料科学 · 电化学 · 表面科学
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MINERALS ENGINEERING · 2026 · IF 6

New insights into the effect of differences in copper sites on the selective separation of CuFeS2 and MoS2 in Cu2+-containing systems

Wentao Li,Hongxiang Xu,Erfeng Zhang,Zechao Huangfu,Jiushuai Deng

Copper site differences determine CuFeS 2 –MoS 2 flotation selectivity in Cu 2+ -containing systems. • ADT forms chelate coordination with surface Cu sites but not lattice Cu sites. • Monodentate ligands provide better CuFeS 2 –MoS 2 separation than bidentate ligands in Cu 2+ -containing systems. Interfaces involving Cu 2+ solutions play a critical role in CuFeS 2 -MoS 2 separation, and the differences among copper sites at the atomic scale are essential for understanding and controlling their separation in Cu 2+ -containing systems. Herein, sodium thioglycolate (STC) and amidinothiourea (ADT) were selected to systematically investigate the effects of copper site differences and inhibitor coordination modes on the selective separation of CuFeS 2 and MoS 2 in Cu 2+ -containing systems. The results suggest that the copper sites within the crystal lattice may be unable to form chelate rings with ADT, possibly due to geometric constraints imposed by the lattice coordination environment. In contrast, coordinated copper sites on the surface of CuFeS 2 may form chelate rings with ADT, thereby enhancing the inhibitory effect. The coordinated copper sites on the surface of MoS 2 may also exhibit a strong affinity for ADT, which hinders the selective separation of CuFeS 2 and MoS 2 . In comparison, STC exhibited a relatively weaker inhibitory effect on MoS 2 . Therefore, selecting reagents with appropriate structures may mitigate the adverse effects of Cu 2+ to some extent. These results suggest that monodentate ligand-based inhibitors containing multiple polar functional groups could be promising candidates for CuFeS 2 -MoS 2 separation in Cu 2+ systems. In addition, since Cu 2+ adsorbs more strongly to the surface of CuFeS 2 than to MoS 2 , and in combination with the control of Cu 2+ concentration, it is expected that the interference from Cu 2+ can be further reduced. This study provides new insights into the selection and design of MoS 2 -CuFeS 2 separation inhibitors in Cu 2+ -containing systems. Download: Download high-res image (300KB) Download: Download full-size image

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JOURNAL OF SOLID STATE ELECTROCHEMISTRY · 2025 · IF 2.6

Preparation of CoS1.097-NiS-MoS2 battery-type electrode material by sulfuration of ZIF-67/NiMoO4 for hybrid supercapacitor application

Xiao Feng,Wang Lei,He Qihang,Xu Fan,Wu Donghua,Chen Chao,He Ping,Tang Bin

Designing promising electrode material for supercapacitor application with rich redox activities, high capacity and great cycling stability has become a research priority. Herein, a nanohybrid (CoS 1.097 -NiS-MoS 2 ) with nanosheets combining nanorods morphology is prepared by high-temperature pyrolysis sulfuration of ZIF-67/NiMoO 4 . Co-existence of multiple crystalline phases is favorable for enriching electrochemical active sites and facilitating electron transfer. Consequently, CoS 1.097 -NiS-MoS 2 displays better supercapacitor performance with a specific capacity of 373.6 C g −1 at current density of 1 A g −1 and excellent cycling stability of 70.01% after 3000 cycles, surpassing CoS 1.097 (49.1 C g −1 ; 59.26%) and NiS-MoS 2 (105.8 C g −1 ; 62.00%). Moreover, a hybrid supercapacitor is assembled with CoS 1.097 -NiS-MoS 2 and activated carbon, exhibiting high energy density of 21.0 Wh kg −1 at 800 W kg −1 . This work opens a path for preparation of promising ternary metal sulfide-based materials for the field of energy storage.

CAS / MDL: 693-98-1 2114-02-5
研究领域: 材料科学 · 电化学 · 能量存储 · 纳米技术
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POLYMER INTERNATIONAL · 2021 ·Vol. 71 ·期 1 ·38-46 · IF 2.99

Amidinothiourea-linked covalent organic framework for the adsorption of heavy metal ions

Heping Wang,Bang Feng,Qianwen Zhang,Qiang Du,Qiuhong Bai,Cong Li,Yehua Shen

For the first time, a novel amidinothiourea-linked covalent organic framework (COF) (TpAt) has been successfully synthesized by the condensation between 1,3,5-triformylphloroglucinol and amidinothiourea via vacuum solvothermal reaction, and was further utilized for the adsorption of metal ions from aqueous solution. The effects of initial concentration, pH and contact time on the adsorption process were investigated. As a result, the TpAt COF showed maximum binding capacities as high as 95.44, 100.76 and 99.08 mg g –1 for Cr(III), Cd(II) and Cu(II) within 180 min at the initial concentration of 100 mg L –1 , respectively. The isotherms of metal ions onto TpAt could be described by the Freundlich isotherm equation, and the adsorption kinetics followed the pseudo-second-order model. The TpAt could be reused for more than five adsorption–elution cycles, whilst basically maintaining its original adsorption performance and the structural integrity of the COF layers. The robust adsorption efficiency can be attributed to the coordination between metal ions and N, O and S atoms in the TpAt framework. The TpAt COF represents an ideal candidate for the removal of heavy metal ions in environmental pollution treatment. © 2021 Society of Industrial Chemistry.

研究领域: 材料科学 · 环境科学
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JOURNAL OF HAZARDOUS MATERIALS · 2019 · IF 7.65

Functional group-rich hyperbranched magnetic material for simultaneous efficient removal of heavy metal ions from aqueous solution

Huicai Wang,Zhenwen Wang,Ruirui Yue,Feng Gao,Ruili Ren,Junfu Wei,Xiaolei Wang,Zhiyun Kong

In order to achieve the purpose of simultaneous removal of coexisting heavy metal ions, in this work, functionalized magnetic mesoprous nanomaterials (Fe 3 O 4 -HBPA-ASA) with high density and multiple adsorption sites were designed and prepared. The obtained Fe 3 O 4 -HBPA-ASA was characterized by SEM, FTIR, VSM, TGA and zeta potential. Cu(II), Pb(II) and Cd(II) were chosen as the model heavy metal ions, the adsorption experiments showed that Fe 3 O 4 -HBPA-ASA showed hightheoretical adsorption capacitiesin individual system, and the maximum adsorption capacity was 136.66 mg/g, 88.36 mg/g and 165.46 mg/g, respectively. In the binary and ternary systems, the competitive adsorption leads to a decrease in the adsorption capacity of Cu(II), Pb(II) and Cd(II). However, in the ternary system with a concentration lower than 15 mg/L, the simultaneous removal rate was still higher than 90%. The adsorption isotherms and kineticswere well fitted by Langmuir and pseudo-second-order models, respectively. The XPS and density functional theory (DFT) analysis have confirmed that the adsorption of metal ions was related to various types of functional groups on the surface of Fe 3 O 4 -HBPA-ASA, while the adsorption mechanisms of Cu(II), Cd(II) and Pb(II) were different.

研究领域: 环境科学 · 材料科学
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Molecular Catalysis · 2019 · IF 2.938

Facile synthesis of zinc halide-based ionic liquid for efficient conversion of carbon dioxide to cyclic carbonates

Chaokun Yang,Yanglin Chen,Ping Xu,Li Yang,Jiaxu Zhang,Jianmin Sun

Multifunctional monocomponent zinc halide-based ionic liquids, amidinothiourea-ZnI 2 (ATUI) and N-phenylthiourea-ZnI 2 (NTUI), were facilely developed as homogeneous catalysts for efficient conversion of CO 2 with epoxides to cyclic carbonates. On account of synergistic effects of multifunctional components in ATUI, the propylene carbonate yield could reach 95% under 110 °C, 1.0 MPa, 4.0 h or even mild conditions. There was a slight decrease of propylene carbonate yield because of the loss of ATUI during the reuse process. Additionally, the universality of ATUI was also studied to other terminal epoxides. Meanwhile, a plausible reaction mechanism was proposed where the synergistic effects involving cation structure and halogen anion of ATUI guarantee the cycloaddition reaction to proceed effectively under solvent and co-catalyst free condition. Finally, reaction kinetics were undertaken to compare the catalytic efficiency of ATUI and NTUI so as to compare the catalytic activity of different numbers of hydrogen bond donor in amidinothiourea and N-phenylthiourea.

研究领域: 化学 · 材料科学 · 环境科学
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Nano Research · 2021 ·Vol. 15 ·期 4 ·2928-2934 · IF 8.897

Constructing Pd-N interactions in Pd/g-C3N4 to improve the charge dynamics for efficient photocatalytic hydrogen evolution

Xiao Xudong,Lin Siying,Zhang Liping,Meng Huiyuan,Zhou Jing,Li Qi,Liu Jianan,Qiao Panzhe,Jiang Baojiang,Fu Honggang

The formation of chemical bonds between metal ions and their supports is an effective strategy to achieve good catalytic activity. However, both the synthesis of active metal species on a support and control of their coordination environment are still challenging. Here, we show the use of an organic compound to produce tubular carbon nitride (TCN) as a support for Pd nanoparticles (NPs), creating a composite material (NP-Pd-TCN). It was found that Pd ions preferentially bind with the electron-rich N atoms of TCN, leading to strong metal-support interactions that benefit charge transfer from g-C 3 N 4 to Pd. X-ray absorption spectroscopy further revealed that the metal-support interactions resulted in the formation of Pd-N bonds, which are responsible for the improvement in the charge dynamics as evidenced by the results from various techniques including photoluminescence (PL) spectroscopy, photocurrent measurements, and electrochemical impedance spectroscopy (EIS). Owing to the good dynamical properties, NP-Pd-TCN was used for photocatalytic hydrogen evolution under visible-light irradiation ( λ > 420 nm) and an excellent evolution rate of ∼ 381 µmol·h −1 (0.02 g of the photocatalyst) was attained. This work aims to promote a strategy to synthesize efficient photocatalysts for hydrogen production by controllably introducing metal nanoparticles on a support and in the meantime forming chemical bonds to achieve intimate metal-support contact.

研究领域: 材料科学 · 化学
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Effect of heteroatom doping on the charge storage and operating voltage window of nickel-based sulfide composite electrodes in alkaline electrolytes

Fangxiang Song,Xianquan Ao,Qianlin Chen

Broadening the voltage window of nickel-based sulfide composite electrodes in alkaline electrolytes is enormously challenging. In prior work, the voltage window of nickel-based sulfide composite electrodes was broadened to 1.8 V (−0.5–1.3 V. vs SCE). Herein, the voltage window widening mechanism of nickel-based sulfide composite electrodes in alkaline electrolytes is discussed in detail. Our results show that co-doped boron and nitrogen atoms and sulfur vacancies increase the number of electrochemical energy storage sites and accelerate the electrochemical reaction, thereby enhancing charge storage. Additionally, heteroatom doping and the presence of sulfur vacancies can effectively inhibit the water decomposition reaction, broadening the voltage window of nickel-based sulfide composite electrodes in alkaline electrolytes and even exceeding the thermodynamic limit of water. Introducing a mesoporous structure increases the electrolyte storage space, accelerating the OH − transfer and charge transfer dynamics. Aqueous and all-solid-state asymmetric supercapacitor devices are assembled, and at a power density of 1800 W kg −1 , the aqueous asymmetric device can obtain a high energy density of 56 Wh kg −1 . The all-solid-state asymmetric device shows a high energy density of 49.72 Wh kg −1 at a power density of 1000 W kg −1 . A theoretical basis is provided for preparing high-energy nickel-based sulfide supercapacitors with a wide voltage window.

CAS / MDL: 2114-02-5
研究领域: 材料科学 · 电化学 · 能源存储
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MATERIALS CHEMISTRY AND PHYSICS · 2023 · IF 4.6

Thiol -functionalized activated carbon fibers as efficient adsorbents for Pb2+

Zhu Lingkai,Xi Man,Yao Yuyuan,Lan Ping

In this study, thiol functionalized activated carbon fibers (ACF-SH) are employed to improve adsorption performances of heavy metals, resulting high density of sulfur-containing and nitrogen-containing groups (6.64 atom % S, 4.49 atom % N confirmed by X-ray Photoelectron Spectroscopy, XPS) and high binding affinity towards Pb 2+ . We find that time, pH, initial ion concentration and adsorbent dosage are important factors affecting the adsorption capacity of modified activated carbon fibers for Pb 2+ . The kinetics and isotherm studies show that the pseudo-second-order model and Langmuir isotherm model can more reasonably explain the adsorption mechanism. Excitingly, the q max obtained through Langmuir isotherm model reaches 700.77 mg g −1 , which significantly surpassed most fiber-based adsorbents. Thermodynamic results significantly exhibit positive ΔH θ and ΔS θ indicating the endothermic property during Pb 2+ adsorption onto ACF-SH with an increase, and a negative ΔG θ reveals its spontaneous at the same time. Moreover, the adsorption mechanism is revealed by diversified analysis. The outcomes from this work indicate that the activated carbon fibers are promising as an adsorbent for effectively repairing Pb 2+ ions in effluent.

研究领域: 环境科学 · 材料科学 · 化学工程
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Journal of Environmental Chemical Engineering · 2023 · IF 7.7

The design and adsorption behaviors study of Pd(II) removal materials deriving from quantitative electron transfer ratio evaluation

Lulu Zhang,Long Jiang,Yaojie Liu,Zongjiang Yu,Ximin Chen,Xiaomeng Su,Mo Xian,Weizhi Sun,Chao Xu

Currently searching for effective noble metal separation material is generally blind and time-consuming. Although theoretical calculation has been widely applied to explain the adsorption mechanism, the quantitative coordination effect between ligand and metal remains to be explored especially in the material screening stage. In this study, Pearson’s theory and Koopmans' theory were used to calculate the electron transfer ratio (ΔN) from different ligands containing N, S, and O to PdCl 2 . The quantitative evaluation contributed to the design of efficient ligands including EA (ΔN =0.5929), DB (ΔN =0.5483), and AT (ΔN =0.4885). And the corresponding polystyrene materials CMPS-EA, CMPS-AT, CMPS-DB were successfully synthesized via chemical modification. According to the adsorption experiment, the per mmol of ligand adsorption capacity from CMPS-EA, CMPS-DB and CMPS-AT for Pd(II) were 0.67 mmol/mmol, 0.17 mmol/mmol and 0.11 mmol/mmol, respectively, exhibiting a positive correlation with the results of ΔN. Moreover, CMPS-EA could efficiently remove 98.01% Pd(II) in the presence of multiple competing metal ions with five times concentration higher than Pd(II). In column study, the breakthrough point (C t /C 0 =0.05) for CMPS-EA was 666–676 BV in 1 mmol/L Pd(II) solution and up to 95% desorption efficiency within 50 BV. The adsorption differences and mechanism of CMPS-EA, CMPS-AT and CMPS-DB were further investigated by FTIR, XPS, ESP, and NBO.

研究领域: 化学工程 · 材料科学 · 环境科学
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