Inorganic Chemistry Frontiers
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2017
·Vol. 5
·期 1
·258-265
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IF 4.036
Lili Tan,Yanhong Liu,Baodong Mao,Bifu Luo,Guan Gong,Yuanzhi Hong,Biyi Chen,Weidong Shi
The development of single-component photocatalysts with narrow bandgaps (2.0–3.0 eV) has been one of the most important goals for photocatalytic H2 production, for which I–III–VI multinary sulfides play an important role due to their widely tunable composition-dependent bandgap. However, simultaneous bandgap narrowing and photocatalytic activity enhancement in the I–III–VI sulfides are often difficult to achieve due to increased defect states. Here, a series of Cu–In–Zn–S quantum dots (QDs) were synthesized by a facile hydrothermal method focusing on a more profound understanding of bandgap tuning and the subsequent effect on the photocatalytic process by controlling the Cu content. The bandgap of the QDs can be effectively tuned from 2.90 eV to 1.98 eV with an increasing Cu : In ratio from 0.05 : 10 to 2.5 : 10 and a color change from light yellow to dark red. The QDs show photocatalytic H2 production activity even without any cocatalyst, but it quickly starts to decrease with the Cu/In ratio over 0.1 : 10 (bandgap of 2.59 eV), which highly limits the potential for visible light photocatalysis. Interestingly, Pt-loading effectively enhanced not only the tolerance of Cu incorporation, but also enabled a high H2 production activity even with further bandgap narrowing down to ∼2 eV. The best photocatalytic performance of 456.4 μmol h−1 g−1 was achieved for the Cu : In : Zn ratio of 1 : 10 : 5 with a bandgap of 2.27 eV. This increased tolerance of Cu content may result from a combined effect of charge separation by Pt as the cocatalyst that alleviated the Cu-induced charge recombination. The enhanced charge separation was proved by the photoluminescence quenching of the QDs with the cocatalyst. Electrochemical impedance spectroscopy was further used to study the charge separation properties of this photocatalytic system. This is the first observation of the cocatalyst-enhanced tolerance of Cu resulting from the competition of cocatalyst-induced charge separation and defect-induced charge recombination in multinary sulfides, which provides an interesting view and design guideline for the development of narrow bandgap photocatalysts.
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ACS Applied Materials & Interfaces
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2014
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IF 5.9
Yanchun Yang,Gang Wang,Wangen Zhao,Qingwen Tian,Lijian Huang,Daocheng Pan
Solution deposition approaches play an important role in reducing the manufacturing cost of Cu2ZnSnSe4 (CZTSe) thin film solar cells. Here, we present a novel precursor-based solution approach to fabricate highly efficient CZTSe solar cells. In this approach, low-cost elemental Cu, Zn, Sn, and Se powders were simultaneously dissolved in the solution of thioglycolic acid and ethanolamine, forming a homogeneous CZTSe precursor solution to deposit CZTSe nanocrystal thin films. Based on high-quality CZTSe absorber layer, pure selenide CZTSe solar cell with a photoelectric conversion efficiency of 8.02% has been achieved without antireflection coating.
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NEW JOURNAL OF CHEMISTRY
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2017
·Vol. 41
·期 9
·3308-3319
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IF 3.269
Qiang Jia,Yinxian Peng,Jianming Pan,Xiaobin Huang,Xiangheng Niu,Tao Zhang
Magnetic microspheres (Fe3O4@PVIM@Zn(II)) composed of a high magnetic-response Fe3O4 core and a Zn(II)-immobilized cross-linked polyvinyl imidazole (PVIM) shell via reflux-precipitation polymerization and metal-ion affinity strategy were fabricated. Integrating the advantages of specific uptake and fast separation, Fe3O4@PVIM@Zn(II) was adopted as an ideal pathway for luteolin (LTL) recognition. As-prepared Fe3O4@PVIM@Zn(II) possessed core–shell structure, uniform size (200 nm), high magnetic responsiveness (32.6 emu g−1), and a very easy synthesis process. X-ray photoelectron spectroscopy (XPS) suggested a strong interaction between the nitrogen heterocyclic ring of PVIM and Zn(II), which produced abundant binding sites for LTL. The batch mode experiments can be well described by pseudo-first-order kinetic models and a Langmuir isotherm. A rapid binding equilibrium (within 45 min) and large monolayer adsorption capacity (23.92 mg g−1) at 298 K were also observed. In addition, Fe3O4@PVIM@Zn(II) displayed remarkable selectivity to LTL; the purification process using Fe3O4@PVIM@Zn(II) can make purified LTL from approximately 85% to 94.26%. The antibacterial activity of purified LTL was outstanding by means of a Staphylococcus aureus (ATCC29213) resistance experiment. Considering its multiple merits, Fe3O4@PVIM@Zn(II) exhibited great potential for specific binding with natural products, such as flavonoids.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Jin Yue,Sun Liping,Wang Yuechen,Huo Lihua,Zhao Hui
Electrocatalytic nitrate reduction reaction (NO 3 RR) provides a promising method for ammonia (NH 3 ) producing. It is urgent to develop efficient catalysts with improved NO 3 RR performance. In this paper, Cu 3 P@Co(OH) 2 /CF heterostructure catalyst is constructed by electrodeposition of cobalt hydroxide (Co(OH) 2 ) nanosheet on the surface of copper phosphide (Cu 3 P) nanorod , and used as a self-supporting cathode for electrocatalytic reduction of nitrate to ammonia. The NH 3 yield reaches 0.19 mmol h −1 cm −2 at a potential of −0.17 V vs. RHE, and the faraday efficiency (FE) is 86.7 %. The study manifests that the built-in electric field generated at the p-n heterojunction interface optimizes the electron migration kinetics, and promotes the adsorption of nitrate and the convention of intermediate product NO 2 − into ammonia. As a consequence, the selectivity of NH3 is improved. The Zn-nitrate battery is assembled with the designed catalyst as the cathode, to reach a peak power density of 5.16 mW cm −2 . The prepared catalyst realizes three effective functions: power output, ammonia synthesis , and nitrate pollutants treatment.
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FUEL
·
2024
·
IF 6.7
Zhengyuan Jin,Yangsen Xu,Bin Xue,Luhong Zhang,Xinzhong Wang,Nayab Arif,Muhammad Ahsan Iqbal,Lu Qi,Yu-Jia Zeng,Teruhisa Ohno
Photocatalytic water splitting has emerged as a vital technology for producing clean hydrogen fuel, addressing global energy needs. However, most research has focused on half-water splitting with sacrificial agents, which limits its practical application in fuel production. In this study, we present an advanced co-catalyst system for polymeric carbon nitride (CN) designed for efficient overall water splitting, a crucial step toward scalable hydrogen fuel generation. The co-catalyst system includes full loading of CoO x , Zn-Pt, and Cr 2 O 3 , with Zn strategically inserted between Pt and CN. This configuration enhances the spatial separation of photoexcited carriers, promoting efficient segregation of oxidation and reduction sites while minimizing electron-hole recombination. The optimized system achieves a stoichiometric H 2 and O 2 ratio of 2:1, with a hydrogen evolution rate that is nine times higher than when Pt alone is used as the co-catalyst. This advancement provides a pathway for efficient solar-driven hydrogen production, addressing the critical challenge of moving beyond half-water splitting and contributing to the development of clean fuel technologies.
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SOLAR ENERGY MATERIALS AND SOLAR CELLS
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2024
·
IF 6.3
Jianbo Ren,Tao Hu,Wenbo Zhang,Li Li,Wenhui Yuan
Photothermal phase change materials (PCM) are employed for the efficient conversion and storage of solar energy. In this work, a Cu-Zn bi-metallic metal-organic framework (MOF) was synthesized and combined with expanded graphite (EG), followed by high-temperature carbonization to prepare the supporting material for polyethylene glycol (PEG). Through the high-temperature carbonization process, nano-metallic copper is uniformly dispersed on the surface of the EG, accompanied by the formation of a new porous structure resulting from the evaporation of Zn vapour. The nano metallic copper particles enhance the thermal conductivity and photo-thermal conversion efficiency of the composite PCM, while the porous structure generated by Zn vapour improves the adsorption capacity of PEG. The composite PCM demonstrated a high phase change enthalpy of 174.6 J/g and excellent thermal reliability, with only a 2.29 % reduction in enthalpy after 200 melting-freezing cycles. Additionally, the thermal conductivity of the composite PCM reached 6.096 W/(m·K) which is 26.1 times higher than that of pure PEG, while the photo-thermal conversion efficiency achieved was 88.69 %. These properties indicate that the PEG/EG/Cu-Zn-MOF derived carbon composite PCM has great potential for applications in solar energy storage and conversion.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Shaosheng Rao,Yangyang Sun,Juan Xie,Chenglong Chen,Chuang Zhi,Rong Ma,Qinqin Liu,Juan Yang
Although photocatalytic disinfection can avoid secondary pollution and other shortcomings compared to traditional disinfection methods, its development is seriously hindered by poor charge separation and transfer efficiency. Herein, we design a Zn-NC (single Zn atoms embedded in nitrogen-doped carbon) bridged ZnO/C 3 N 4 Z-scheme heterojunction (ZnO/Zn-NC/C 3 N 4 ) with robust interface contact by a multi-interfacial engineering strategy to achieve highly efficient separation and transfer of charge. Experimental and theoretical analyses demonstrate that the tightly integrated interface and excellent electrical conductivity of Zn-NC electron bridges ensure effective transfer of photogenerated charge carriers. Compared to ZnO/C 3 N 4 , the introduction of Zn-NC electron bridges induces charge rearrangement at the interface, generating a strong built-in electric field in the ZnO/Zn-NC/C 3 N 4 Z-scheme heterojunction to facilitate the separation and transfer of photogenerated charge carriers. Furthermore, Zn-NC electron bridges effectively promote the adsorption and activation of oxygen on the surface of ZnO/Zn-NC/C 3 N 4 , enhancing the generation of reactive oxygen species for rapid bacteria elimination in water. Consequently, the ZnO/Zn-NC/C 3 N 4 Z-scheme heterojunction, at a concentration of 100 ppm, achieves 99.9 % antibacterial efficiency against methicillin-resistant Staphylococcus aureus , Staphylococcus aureus , and Escherichia coli at a bacterial concentration of ∼ 10 7 CFU/mL under AM 1.5G simulated sunlight irradiation for 60 min, which is approximately 1.05 times higher than that of ZnO/C 3 N 4 . Moreover, ZnO/Zn-NC/C 3 N 4 maintains a 99.9 % bactericidal efficiency for natural water treatment using a homemade microreactor, demonstrating its potential for water disinfection.
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FUEL
·
2024
·
IF 6.7
Juzhi Leng,Xinru Yang,Qi Zeng,Wenting Chen,Shupeng Guo,Min Zhong,Lili Liu,Yunlei Chen,Pengju Yang,Mingqi Li
Photochemical reduction of CO 2 (CO 2 RR) to syngas is an attractive approach for carbon–neutral recycling. Manipulating binding strength to reactive species on catalyst surfaces is challenging but essential for achieving efficient syngas production with a desired CO/H 2 ratio. Here, we demonstrate that the binding strength to key reaction intermediates (*CO 2 , *H and *CO) on the Co 3 O 4 surface can be fine-tuned by incorporating varying amount of Zn atoms. Dedicated experiments and theoretical simulations unveil that Zn doping allows for simultaneous control of both CO 2 adsorption/activation and the adsorption affinity of *CO on Zn-Co 3 O 4 catalysts, resulting in a significant enhancement in CO 2 to CO conversion. Moreover, Zn doping can alter the hydrophilicity of the catalyst surface, affecting the water adsorption behavior and adjusting the hydrogen evolution reaction (HER) activity. As a result, the CO/H 2 ratio can be readily tuned via varying the Zn doping level. This study presents an effective and economical method approach to manipulate the electronic structure of catalyst surfaces for controlling the kinetics of CO 2 RR and HER reactions, providing valuable insight into the design of highly active transition metal oxides (TMOs) based photocatalysts for syngas production with a tailored CO/H 2 ratio.
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ELECTROCHIMICA ACTA
·
2024
·
IF 5.5
Jiaheng Wang,Fengxiang Yang,YuChen Wang,Yang Zhao,Wei Wang,Anchun Fang,Songyuan Wu,Qingwei Wang,Jiarui Li,Jiaxu Gong,Yatang Dai
It remains an urgent task to design electrocatalysts with fast oxygen evolution reaction (OER) kinetics and enriched active sites for flexible Zn-air batteries. In this paper, a structure engineering strategy is proposed to design an electrocatalyst with a heterostructure comprising Co@NC and NiMo-LDH on carbon cloth, which serves as an air electrode for a quasi-solid-state Zn-air battery. This unique heterostructure significantly enhances electrocatalytic activity, producing low OER overpotentials of 198 mV at 10 mA cm -2 . Moreover, the assembled rechargeable Zn-air battery exhibits a high peak density and long cycle stability. Density functional theory calculations indicate that the multimetallic heterostructure induced synergistic and electronic coupling effects among the metal active sites, facilitating rapid ion and electron transport during the OER process. In addition, the migration of oxygen species at the Ni and Mo sites reduces the reaction potential barrier, resulting in a low OER overpotential of 160 mV.
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Small
·
2024
·
IF 13
Yuexin Liu,Jing Zhang,Yuan Liu,Mingcheng Zhang,Zhenghui Pan,Kefeng Cai
Introducing N atoms in vanadium oxides (VO x ) of aqueous Zn-ion batteries (ZIBs) can reduce their bandgap energy and enhance their electronic conductivity, thereby promoting the diffusion of Zn 2+ . The close-packed vanadium oxynitride (VON) generated often necessitates the intercalation of water molecules for restructuring, rendering it more conducive for zinc ion intercalation. However, its dense structure often causes structural strain and the formation of by-products during this process, resulting in decreased electrochemical performance. Herein, carbon-coated porous V 2 O 3 /VN nanosheets (p-VON@C) are constructed by annealing vanadium metal-organic framework in an ammonia-contained environment. The designed p-VON@C nanosheets are efficiently converted to low-crystalline hydrated N-doped VO x during subsequent activation while maintaining structural stability. This is because the V 2 O 3 /VN heterojunction and abundant oxygen vacancies in p-VON@C alleviate the structural strain during water molecule intercalation, and accelerate the intercalation rate. Carbon coating is beneficial to prevent p-VON@C from sliding or falling off during the activation and cycling process. Profiting from these advantages, the activated p-VON@C cathode delivers a high specific capacity of 518 mAh g −1 at 0.2 A g −1 and maintains a capacity retention rate of 80.9% after 2000 cycles at 10 A g −1 . This work provides a pathway to designing high-quality aqueous ZIB cathodes.
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ACS Applied Energy Materials
·
2025
·
IF 5.5
Dongheng Zhao,Qian Ma,Ying Sun,Lingyu Li,Huayushuo Zhang,Bolong Li,Zhiqiang Liu,Xiaomei Jiang
Zero-dimensional organic zinc halides have garnered significant attention as efficient and eco-friendly photoluminescent materials. However, its luminance efficiency, which is typically attributed to self-trapped excitons formed within zinc halide tetrahedra, often encounters a serious thermal quenching problem. This issue significantly limits its application in the field of solid-state lighting. Intriguingly, the incorporation of tetra-coordinated Mn2+ ions into these organic zinc halides can effectively mitigate unnecessary electron interactions and nonradiative energy transfer between Mn–Mn, achieving significantly improved photoluminescence quantum yield (PLQY) in the alloyed materials. In this work, a series of zero-dimensional Mn2+-alloyed 4-benzylpiperidinum zinc chloride hybrids were designed and synthesized by a solvent evaporation method. It is noteworthy that the pure zinc chloride shows a negligible visible emission at 510 nm, whereas (C12H12N)2MnxZn1–xCl4 (x = 0.25, 0.5, 0.75, 1) emits visible light ranging from green to yellow at room temperature. Incorporating Mn has led to a remarkable enhancement in PLQY, increasing from a mere 4.02% in the organic zinc halide to an impressive 94.45% in the (C12H12N)2Mn0.75Zn0.25Cl4. The white LED was successfully fabricated by employing the optimal sample as a single-component yellow phosphor coated on 450 nm chip. The correlated color temperature was determined to be 4770 K with a color rendering index as high as 91. It was also demonstrated with good luminous stability under different working currents. This research provides a straightforward approach for developing eco-friendly, cost-effective, and high-performance single-component yellow phosphors for white LED applications.
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JOURNAL OF POWER SOURCES
·
2024
·
IF 8.1
Shihang Guo,Lin Wang,Chenyang Xue,Sumei Lin,Tingxuan Yi,Yuwen Zhu,Donglin Han
Protonic ceramic cells (PCCs) can convert the energy between electricity and fuels efficiently, and are attracting increasing attention. However, the development of PCCs is restricted by the lack of proper positrode materials. In this work, we report a Co-free system with a nominal composition of BaCe 0.2 Fe 0.8 O 3-δ , which is composed of a Fe-rich matrix phase decorated with Ce-rich nanoparticles. The performance of such a dual-phase positrode system is further improved by doping Zn and/or Ni to increase bulk and surficial concentration of oxygen vacancies. The hydration reaction and surficial adsorption of oxygen species are thereby promoted, benefitting the oxygen reduction reaction. The Ni and Zn co-doped composition Ba(Ce 0.2 Fe 0.8 ) 0.85 (Ni 0.5 Zn 0.5 ) 0.15 O 3-δ exhibits lower polarization resistance than the pristine and singly doped systems, enabling the fuel cells to show high peak power densities of 400, 721, and 828 mW cm −2 at 550, 600, and 650 °C, respectively.
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