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A cyanide-bridged di-manganese carbonyl complex that photochemically reduces CO <sub/>2</sub> to CO
摘要: A cyanide-bridged di-manganese carbonyl complex that photochemically reduces CO2 to CO? Hsin-Ya Kuo, Tia S. Lee, An T. Chu, Steven E. Tignor, Gregory D. Scholes and Andrew B. Bocarsly* Manganese(I) tricarbonyl complexes such as [Mn(bpy)(CO)3L] (L = Br, or CN) are known to be electrocatalysts for CO2 reduction to CO. However, due to their rapid photodegradation under UV and visible light, these monomeric manganese complexes have not been considered as photocatalysts for CO2 reduction without the use of a photosensitizer. In this paper, we report a cyanide-bridged di-manganese complex, {[Mn(bpy)(CO)3]2(μ-CN)}ClO4, which is both electrocatalytic and photochemically active for CO2 reduction to CO. Compared to the [Mn(bpy)(CO)3CN] electrocatalyst, our CN-bridged binuclear complex is a more efficient electrocatalyst for CO2 reduction using H2O as a proton source. In addition, we report a photochemical CO2 reduction to CO using the dimanganese complex under 395 nm irradiation.
关键词: electrocatalyst,cyanide-bridged,photochemical reduction,CO2 reduction,di-manganese,photocatalyst,carbonyl complex
更新于2025-11-19 16:56:42
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Thiourea-assisted coating of dispersed copper electrocatalysts on Si photocathodes for solar hydrogen production
摘要: Photoelectrochemical water splitting can convert solar energy into clean hydrogen energy for storage. It is desirable to explore non-precious electrocatalysts for practical applications of a photoelectrode in a large scale. Here, we developed a facile spin-coating and in-situ photoelectrochemical reduction method to prepare a dispersed Cu electrocatalyst on a Si photocathode, which improves the performance remarkably. We find that thiourea in the precursor solution for spin-coating plays an important role in obtaining dispersed Cu particles on the surface of a Si photoelectrode. With thiourea in the precursor, the Cu/Si photocathode shows higher performance than the one without thiourea. Moreover, the Cu/Si photocathode also indicates good stability after 16 h illumination.
关键词: In-situ photoelectrochemical reduction,Cu electrocatalyst,Thiourea,Hydrogen evolution reaction
更新于2025-11-19 16:51:07
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Defective ZnS nanoparticles anchored in situ on N-doped carbon as a superior oxygen reduction reaction catalyst
摘要: Defect engineering has been used to develop low-cost and effective catalysts to boost oxygen reduction reactions. However, the development of catalysts that use metal cation vacancies as the active sites for oxygen reduction reaction is lacking. In this study, ZnS nanoparticles on N-doped carbon serve as an oxygen reduction reaction catalyst. These catalysts were prepared via a one-step method at 900 °C. Amazingly, the high-resolution transmission electron microscope image revealed obvious defects in the ZnS nanoparticles. These facilitated the catalyst synthesis, and the product displayed good electrocatalytic performance for the oxygen reduction reaction in an alkaline medium, including a lower onset potential, lower mid-wave potential, four electron transfer process, and better durability compared with 20 wt% Pt/C. More importantly, the density functional theory results indicated that using the Zn vacancies in the prepared catalyst as active sites required a lower reaction energy to produce OOH ? from ?OO toward oxygen reduction reaction. Therefore, the proposed catalyst with Zn vacancies can be used as a potential electrocatalyst and may be substitutes for Pt-based catalysts in fuel cells, given the novel catalyst’s resulting performance.
关键词: Density functional theory calculations,Oxygen reduction reaction,Zn vacancy,Electrocatalyst,Defective ZnS nanoparticle
更新于2025-11-14 17:03:37
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CePd‐Nanoparticles‐Incorporated Carbon Nanofibers as Efficient Counter Electrode for DSSCs
摘要: In this study, the cerium-palladium (CePd) incorporated carbon nanofibers (CNFs) were manufactured by low-cost and versatile electrospinning technique and successfully applied as a counter electrode to fabricate the dye-sensitized solar cells (DSSCs). The utilized physiochemical techniques, X-ray diffractometer (XRD), X-ray photoelectron spectroscopy (XPS), field-emission scanning electron microscope (FESEM), and transmission electron microscope (TEM) confirmed the formation of carbon nanofibers (CNFs) incorporated by Ce and Pd nanoparticles. CePd incorporated CNFs were preliminary presented good electrocatalytic activity towards the iodide redox couple, as investigated by cyclic voltammetry. The DSSC fabricated using CePd incorporated CNFs based counter electrode (CE) attained an applicable power conversion efficiency (PCE) of 4.52% along with open circuit voltage (VOC) of 0.739 V, a short-circuit current density (JSC) of 11.42 mA/cm2 and fill factor (FF) of 0.54. According to primary results, the CePd incorporated CNFs based CE is a promising, and cost-effective alternative CE for photoelectrochemical devices.
关键词: Alloys nanoparticles,Solar cells,Electrocatalyst,Cyclic voltammetry,Carbon nanofibers
更新于2025-09-23 15:23:52
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2D Schottky Junction between Graphene Oxide and Transition-Metal Dichalcogenides: Photoresponsive Properties and Electrocatalytic Performance
摘要: 2D graphene is conductor and not a semiconductor. 2D transition—metal dichalcogenides (TMD) is a semiconductor and not a conductor. Preparing 2D composite material that simultaneously possesses both advantages of graphene and TMD has proven to be challenging. In this work, both 2D-WS2/2D-GO and 2D-MoS2/2D-GO composites with few layer thickness are synthesized. The electronic structure indicates a high content of Mo4+ 3d5/2 and W4+4f7/2 with lower binding energy in the 2D composite, which is ascribed to partial loss of surface sulfur atoms in 2D composites and the newly formed heteroatomic bond of CWS and CMoS. The Schottky junction between 2D-GO and 2D-TMD (2D G-T junction) is established and exhibits obvious photoelectric responses. Superior electrocatalytic properties of the two 2D-composites are attributable to the 2D Schottky Junction between 2D-TMDs and 2D-GO. Interlayer electronic coupling in 2D Schottky Junction (2D G-T junction) activates inert sites on the 2D surface of 2D-TMDs or GO. The power conversion efficiency of dye-sensitized solar cells (DSCs) based on 2D-WS2/2D-GO is 9.54% under standard solar illumination intensity (AM1.5, 100 mW cm?2). The value is one of the highest reported efficiencies for DSCs based on Pt-free counter electrodes. Finally, 2D-WS2/2D-GO composites exhibit excellent stability as counter electrode of DSCs.
关键词: photoresponse,interlayer electronic coupling,2D,electrocatalyst,graphene,transition-metal dichalcogenides,Schottky junction
更新于2025-09-23 15:23:52
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Reaction Packaging CoSe <sub/>2</sub> Nanoparticles in N-Doped Carbon Polyhedra with Bifunctionality for Overall Water Splitting
摘要: Water electrolysis is a promising approach for green and large-scale hydrogen production; however, there are still challenges for developing efficient and stable bi-functional electrocatalysts towards the hydrogen and oxygen evolution reactions. Herein, zeolitic imidazolate framework-67 (ZIF67) was used as the precursor for the construction of CoSe2 nanoparticles trapped in N-doped carbon polyhedra (NC). Among as-obtained CoSe2-NC hybrid, highly active CoSe2 nanoparticles in sizes of 10-20 nm are encapsulated in N-doped few-layer carbon shell, avoiding their easy aggregations of CoSe2 nanoparticles as well as enhancing the long-term stability. The unique nanostructured CoSe2-NC hybrid with a hierarchical porosity and 3D conductive framework thus fully exerts outstanding bi-functional catalytic activity of CoSe2 centers. As a result, the CoSe2-NC hybrid as bi-functional catalysts for overall water splitting delivers a high current density of 50 mA cm-2 with applied voltage of ~1.73 V in alkaline electrolyte, with a promising stability over 50000 s.
关键词: selenide reaction,ZIF67,bifunctional electrocatalyst,overall water splitting,carbon polyhedra
更新于2025-09-23 15:22:29
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[IEEE 2020 IEEE 33rd International Conference on Micro Electro Mechanical Systems (MEMS) - Vancouver, BC, Canada (2020.1.18-2020.1.22)] 2020 IEEE 33rd International Conference on Micro Electro Mechanical Systems (MEMS) - Graphene Quantum Dots Induced NiCo <sub/>2</sub> S <sub/>4</sub> as an Efficient Electrocatalyst for Hydrogen Harvest
摘要: We made an efficient electrocatalyst for hydrogen harvest, with an overpotential as low as 0.131V to achieve a current density of 10 mA/cm2. The morphology of the material was extremely delicate: branches on the nanowire, and smaller twigs on the branches, such that the specific surface area was greatly enlarged. The two-step hydrothermal process improved performance of is easily accessible. The GQD/NiCo2S4 should mainly be ascribed to graphene quantum dots (GQDs), which induce morphology change of NiCo2S4 nanowires. The delicate morphology serves as a buffer for volume change, and also a reservoir for electrolytes to transport protons [1]. In the meaning time, GQDs inherit excellent properties from both graphene and quantum dots, improving conductivity. Moreover, the addition of GQDs creates numerous defects in both the basal and edge planes for the diffusion of protons and thus help overcome the sluggish redox kinetics of the electrode, leading to improved overall performances [2].
关键词: Hydrogen harvest,Nickel-Cobalt sulfide (NiCo2S4),Electrocatalyst,Graphene Quantum Dots (GQD)
更新于2025-09-23 15:21:01
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Prussian Blue Nanocubesa??SnO <sub/>2</sub> Quantum Dotsa??Reduced Graphene Oxide Ternary Nanocomposite: An Efficient Nona??noblea??metal Electrocatalyst for Nona??enzymatic Detection of H <sub/>2</sub> O <sub/>2</sub>
摘要: Developing non-noble-metal electrocatalyst for non-enzymatic H2O2 sensing is highly attractive. A facile, two-step approach has been utilized for the synthesis of PBNCs/SnO2 QDs/RGO ternary nanocomposite. TEM, SEM, XPS, and XRD techniques were used to the characterize the structural and morphological properties of synthesized ternary nanocomposite. The synthesized ternary nanocomposite has been examined as an electrode material for the electrochemical detection of H2O2 using the Amperometry technique. Under optimum conditions, PBNCs/SnO2 QDs/RGO ternary nanocomposite performed very well in the electrocatalytic reduction of H2O2 with a linear dynamic range from 25-225 μM (R2 = 0.996) with a low detection limit of 71 nM (S/N=3). Compared to the recent literature, PBNCs/SnO2QDs/RGO ternary nanocomposite based modified electrode exhibit a wider linear dynamic range with a low detection limit. Furthermore, PBNCs/SnO2 QDs/RGO ternary nanocomposite based modified electrode showed an excellent anti-interference ability against various common interfering agents. The practical applicability of ternary nanocomposite based modified electrode was further extended to determine the H2O2 in tap water with acceptable recovery. The present performance of PBNCs/SnO2 QDs/RGO ternary nanocomposite material towards H2O2 sensing might widen its application for developing a new type of non-noble metal-based non-enzymatic electrochemical biosensors.
关键词: Hydrogen peroxide,Graphene,Non-enzymatic sensor,SnO2 quantum dots,Non-noble-metal electrocatalyst,Prussian blue nanocubes
更新于2025-09-23 15:21:01
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Oxide-Core Pt-Shell Electrocatalysts for PEFCs: Photochemical Preparation Using SnO <sub/>2</sub> Nanoparticles
摘要: Core-shell electrocatalyst, in which a Pt atomic layer covers a nano-size core of a different metal, is attractive in reducing Pt usage for PEFC cathode electrocatalyst. Whilst such core-shell electrocatalysts exhibit very high mass activity for oxygen reduction reaction (ORR), their cost and durability still remain as a challenge. If inexpensive and thermochemically-stable conductive oxide could be applied to the core instead of a noble metal, cost reduction and durability improvement of such core-shell electrocatalysts may be expected. In this study, we try to develop oxide-core Pt-shell electrocatalysts by directly depositing Pt on SnO2 at an atomic level via a photochemical preparation procedure. SnO2 cores with a diameter down to ca. 3 nm could be prepared by comparing various preparation procedures of SnO2 and types of fillers. Electrochemical activities of such oxide-core Pt-shell electrocatalysts are characterized and discussed.
关键词: PEFC,SnO2,photochemical preparation,Pt-shell,Core-shell electrocatalyst
更新于2025-09-23 15:21:01
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Laser-induced graphene hybrid photoelectrode for enhanced photoelectrochemical detection of glucose
摘要: The combination of electrocatalyst with semiconductor light-absorber is of great importance to increase the efficiency of photoelectrochemical (PEC) glucose detection. Here, in-situ and synchronous fabrication of Ni-based electrocatalyst (NiEC) and CdS semiconductor in laser-induced graphene (LIG) on indium?tin oxide glass is demonstrated via a one-step laser-induced solid phase transition. A series of component and structural characterizations suggest that the laser-induced NiEC uniformly disperses in the hybrid nanocomposite and exists mainly in the form of Ni0 and NiO state. Moreover, both electrochemical and PEC investigations confirm that the as-prepared hybrid photoelectrode exhibits excellent photoelectrocatalytic ability towards glucose, which is not only attributed to the strong synergistic interaction between CdS and NiEC, but also benefited from the high conductivity as well as 3D macroporous configuration of the simultaneously formed LIG, providing the key factor to achieve sensitive non-enzymatic PEC glucose sensors. Therefore, the laser-induced hybrid photoelectrode is then applied to the PEC detection of glucose, and a low detection limit of 0.4 μM is obtained with good stability, reproducibility, and selectivity. This study provides a promising paradigm for the facile and binder-free fabrication of electrocatalyst?semiconductor?graphene hybrid photoelectrode, which will find potential applications in sensitive PEC biosensing for a broad range of analytes.
关键词: nickel electrocatalyst,hybrid nanocomposite,cadmium sulfide,photoelectrochemical sensing,laser-induced graphene,glucose
更新于2025-09-23 15:19:57