| 編號： | 11 |
| 期刊或研討會名稱： |
ChemSusChem
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| 著作名稱： | Electron‐Deficient Bimetallic Oxide Electrocatalyst for High‐Efficiency Ammonia Synthesis Under Ambient Conditions
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| 年度： | 2026 |
| 類別： |
期刊論文
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| 摘要： | Ammonia (NH3) is an essential feedstock for fertilizers and a promising carrier for carbon-free hydrogen fuel. However, its conventional production through the energy-intensive Haber–Bosch process results in significant carbon dioxide emissions. Here, we report an eco-friendly solid-state synthesis of bismuth vanadium oxide supported on treated carbon black (Bi4V6O21@CB), denoted as BV64@CB, as an efficient electrocatalyst for the nitrogen reduction reaction (NRR). This electrocatalyst exhibits exceptional activity owing to its unique coordination environment, which effectively sustains electron deficiencies. In this system, vanadium (V5+) active sites facilitate nitrogen (N2) adsorption, while bismuth (Bi3+) promotes the hydrogenation of adsorbed N2, leading to the formation of *NNH intermediates on the BV64@CB surface. The cooperation between vanadium and bismuth enhances NRR efficiency, thereby promoting NH3 synthesis via the distal associative pathway. These mechanistic insights are supported by in situ X-ray absorption spectroscopy and Raman analyses. The BV64@CB electrocatalyst exhibits an impressive average NH3 yield rate of 370.1 μg h−1 mgcat−1 and a Faradaic efficiency of 90.94% at −0.4 V versus the reversible hydrogen electrode in a 0.2 M Li2SO4 electrolyte (pH 5). This performance surpasses that of other bimetallic oxide electrocatalysts, underscoring its potential as an efficient and sustainable candidate for NH3 synthesis. |
| 關鍵字： | π-back donation | electrocatalysts | electrochemical NRR | Faradaic efficiency | in situ XAS |
| 編號： | 10 |
| 期刊或研討會名稱： |
Electrochimica Acta
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| 著作名稱： | Phthalocyanine-Derived Dual-Atom Nickel Catalysts (Ni-DAC) for Efficient Electrocatalytic CO₂ Reduction
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| 年度： | 2026 |
| 類別： |
期刊論文
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| 摘要： | Electrochemical CO₂ reduction (ECR) is a key route toward carbon-neutral fuel production but remains constrained by the thermodynamic inertness of CO₂, large activation barriers, and competing hydrogen evolution. Nickel phthalocyanine (NiPc) offers well-defined Ni–N₄ centers for CO₂-to-CO conversion, yet suffers from rapid demetallation and macrocycle degradation under cathodic bias, limiting long-term operation. Here, we report a phthalocyanine-derived dual-atom nickel catalyst (Ni-DAC) obtained by controlled thermal restructuring of NiPc into a nitrogen-rich turbostratic carbon matrix that stabilizes synergy-driven Ni–Ni dual centers in concert with unsaturated Ni–N₃ single sites. HAADF-STEM, soft X-ray absorption spectroscopy, and EXAFS unambiguously resolve atomically dispersed Ni–Ni ensembles embedded within the N-doped carbon framework. In 0.5 M KHCO₃, Ni-DAC delivers a CO partial current density of −34 mA cm⁻² with 96.3% Faradaic efficiency at −0.80 V vs RHE, and attains 98.8% CO selectivity at a total current density of 103 mA cm⁻² at −1.20 V, while maintaining stable performance for at least 20 h. Density functional theory reveals that the cooperative Ni₂N₆ motif substantially lowers the free-energy barrier for *COOH formation and facilitates *CO formation and desorption relative to Ni₁N₃/C and Ni–Pc, providing a rigorous mechanistic rationale for the benchmark CO₂-to-CO activity and durability. These findings establish a practical strategy to construct dual-metal M–N–C catalysts from simple metallomacrocyclic precursors and open avenues toward efficient, long-lived CO₂ electrolysis and future C₂+ product generation. |
| 關鍵字： | Dual-atomic catalyst (DAC), Nickel phthalocyanine, CO₂ electroreduction, Ni–N coordination, Faradaic efficiency |
| 編號： | 9 |
| 期刊或研討會名稱： |
Advanced Energy Materials
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| 著作名稱： | Molecular Bottom‐Up Design of Single‐Site Copper‐Palladium Catalysts for Selective Glycerol Electro‐Oxidation
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| 年度： | 2026 |
| 類別： |
期刊論文
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| 摘要： | Hybrid water electrolysis is a promising route to generate hydrogen while replacing the challenging and wasteful oxygen evolution reaction (OER) with economically viable alternatives such as the selective glycerol oxidation reaction (GOR). To date, the development of highly active and selective GOR electrocatalysts remains a major challenge because the simultaneous control of reactivity, selectivity, and stability is difficult. Herein, we report a bimetallic Cu-Pd single-site catalyst (SSC) for the selective and efficient electrooxidation of glycerol. The catalyst features single-site copper and palladium atoms in CuN4/PdN4 moieties. The catalyst shows high GOR performance with a Faradaic efficiency (FE) for formate of 83% and C3 products (lactate, glycolate, glycerate) of 16% at 1.0 V vs the reversible hydrogen electrode (RHE), as well as long-term stability (144 h at j 50 mA cm−2). Mechanistic studies combining DFT and operando spectroscopy revealed that Pd sites facilitate the adsorption of hydroxyl (C-OH) species which prevents C-C bond cleavage and thus the formation of catalyst poisons such as CO or CO32−. This work sheds light on the adsorption modulation mechanism of a single-site catalyst and provides a promising electrocatalytic system for the production of value-added C1 and C3 products in aqueous solution. |
| 關鍵字： | Electrocatalysis| glycerol oxidation reaction| phthalocyanine| single-site catalyst| X-ray absorption spectroscopy |
| 編號： | 8 |
| 期刊或研討會名稱： |
Applied Catalysis B: Environment and Energy
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| 著作名稱： | Host–guest mediated structural tuning of selenium sites in-plane structure of metallic phase tungsten diselenide for enhanced hydrogen production
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| 年度： | 2025 |
| 類別： |
期刊論文
|
| 摘要： | Unconventional synthesis of the metastable 1 T′ phase of transition metal dichalcogenides (TMDs) enhances hydrogen evolution reaction (HER) activity but requires stabilization to prevent its reversion to the 2H phase. To address this, we employed a host–guest interaction-driven strategy to synthesize uniformly Ni-doped 1 T′-WSe2 nanosheets using Anderson-type polyoxometalate (POM) clusters as molecular precursors. This approach ensures homogeneous Ni distribution and promotes phase stability via strong π-type Ni–Se interactions. The optimized Ni-1T′-WSe₂ exhibits significantly enhanced HER performance with lower overpotential. In situ X-ray absorption spectroscopy (XAS) reveals notable Se K-edge shifts in Ni-1T′-WSe2 compared to undoped 1T-WSe2, indicating Ni-induced modulation of Se catalytic sites. Additionally, Ni adsorption of OH* plays a dual role, enhancing water activation and mitigating OH* poisoning effects. Theoretical modeling shows that Ni doping improves charge transfer, stabilizes interstitial Se atoms, and lowers the energy barrier for water dissociation. This work offers key insights into the re-engineering of heteroatom-doped TMDs as promising electrocatalysts for energy conversion applications. |
| 關鍵字： | Metallic phase Hydrogen evolution reaction Electrocatalysis Phase engineering |
| 編號： | 7 |
| 期刊或研討會名稱： |
Chemical Engineering Journal
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| 著作名稱： | Boosting catalytic activity toward industrial water electrolysis: Ag–triggered dual–site activation in NiFe LDH for ultra–efficient oxygen evolution reaction
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| 年度： | 2025 |
| 類別： |
期刊論文
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| 摘要： | Developing efficient and robust nanostructured electrocatalysts is critical in advancing industrial water splitting under large current density (≥500 mA cm−2) with minimal efficiency loss. However, oxygen evolution reaction (OER) catalysts often suffer from huge overpotential and poor long-term stability. Here, we report a silver-promoted, defective NiFe LDH catalyst grown on Ni foam (Ag/a–NiFe LDH/NF), which uncovers outstanding OER activity and durability under commercially relevant current density. The catalyst delivers large current densities of 500 and 1000 mA cm−2 at remarkably low overpotentials of 180 and 220 mV, respectively, while maintaining stable performance over 200 h. Ag/a–NiFe LDH/NF electrodes also demonstrate bifunctional electrocatalytic activity, achieving efficient HER activity and sustained long-term stability for 100 h. Moreover, Ag/a–NiFe LDH/NF enables overall water electrolysis with minimum voltages of 1.67 and 1.76 V at 500 and 1000 mA cm−2, respectively, outperforming the benchmark RuO₂–Pt/C couple. Operando X–ray absorption spectroscopy and in situ Raman spectroscopy reveal that Ag incorporation facilitates the formation of high-valent Ni/Fe oxy–hydroxide active sites. In addition, the introduction of oxygen vacancies and under-coordinated dual-metal sites enhances catalytic activity. Ag atoms enhance electrical conductivity, catalytic activity, accelerate charge transfer, and stabilize the Ni and Fe active structures, thereby synergistically reducing energy barriers for OER. To the best of our understanding, Ag/a–NiFe LDH/NF achieves one of the highest reported OER activities to date under industrial current density. This work offers insights into rational catalyst design for industrial alkaline water electrolysis. |
| 關鍵字： | Water electrolysisLarge current densityDual active sitesOxy–hydroxidesIndustrial electrolyzers |
| 編號： | 6 |
| 期刊或研討會名稱： |
Chemical Engineering Journal
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| 著作名稱： | Decisive electrocatalyst of oxyphilic transition metals with bivalent metal perovskites: Localized oxygen confinement for enhanced 2e-WOR in H2O2 production
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| 年度： | 2025 |
| 類別： |
期刊論文
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| 摘要： | A novel strategy has been developed to boost the efficiency of the electrochemical two-electron water oxidation reaction (2e-WOR) for sustainable, on-site H2O2 production addressing persistent challenges such as low selectivity, high overpotential, and sluggish kinetics. This approach utilizes Sn-based perovskite electrocatalysts (MgSnO3@NF, SrSnO3@NF, CaSnO3@NF, and BaSnO3@NF), synthesized under mild conditions using bivalent metal precursors. The incorporation of oxyphilic A-site cations enhances oxygen intermediate confinement, steering the reaction toward the 2e-pathway. Among them, MgSnO3@NF exhibits superior performance due to the cooperative interaction between Sn and Mg centers with *OH/*O intermediates, enabling a pull-push electronic modulation. It achieves a high Faradaic efficiency of 86.26 %, low onset overpotential (60 mV at 10 mA cm-2), and a notable H2O2 generation rate of 46.26 μmol min-1 cm-2. These enhancements are attributed to accelerated reaction kinetics, increased surface area, and effective suppression of H2O2 decomposition. This work offers a promising route toward selective and durable H2O2 electrosynthesis, presenting a green alternative to traditional anthraquinone and 2e-ORR methods. |
| 關鍵字： | Oxyphilic metal, Confinement, 2e-WOR, H2O2, Local oxygen |
| 編號： | 2 |
| 期刊或研討會名稱： |
Journal of the American Chemical Society
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| 著作名稱： | Heterogeneous Interfaces of Ni3Se4 Nanoclusters Decorated on a Ni3N Surface Enhance Efficient and Durable Hydrogen Evolution Reactions in Alkaline Electrolyte
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| 年度： | 2025 |
| 類別： |
期刊論文
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| 摘要： | Transition metal selenides (TMSes) have been identified as cost-efficient alternatives to platinum (Pt) for the alkaline hydrogen evolution reaction (HER) owing to their distinct electronic properties and excellent conductivity. However, they encounter challenges such as sluggish water dissociation and severe oxidative degradation, requiring further optimizations. In this study, we developed a dual-site heterogeneous catalyst, Ni3Se4–Ni3N, by decorating Ni3Se4 nanoclusters on a Ni3N substrate. This catalyst design promoted significant interfacial electronic interactions, modulated electronic structures, and enhanced the adsorption of the intermediates. Various spectroscopic analyses and theoretical calculations revealed that the nitride surfaces improved water adsorption and dissociation, enriching the surface with adsorbed hydrogen (H*) atoms, while the Se sites facilitated hydrogen coupling and subsequent release of H2. Following a hydrogen spillover mechanism, the surface-adsorbed hydrogen atoms were transferred to nearby electron-dense selenide sites for H2 formation and release. Consequently, the optimized catalyst demonstrated improved HER activity, requiring only an ∼60 mV overpotential at 10 mA cm–2 current density and maintained stability under higher potential conditions. |
| 關鍵字： | |
| 編號： | 3 |
| 期刊或研討會名稱： |
Chemistry of Materials
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| 著作名稱： | Selective Electrochemical Reduction of CO2 to Ethanol on a Heteroatom-Coordinated Dual-Atom Catalyst of Fe/Cu-NC
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| 年度： | 2025 |
| 類別： |
期刊論文
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| 摘要： | Rising CO2 emissions, particularly from industrial sectors, are driving climate change and causing severe environmental and energy crises that demand immediate action. The electrochemical CO2 reduction reaction (eCO2RR) provides a sustainable approach by converting waste CO2 into value-added products. However, achieving a high selectivity for multicarbon products in the eCO2RR requires advanced catalysts with large surface areas, accessible active sites, and strong synergistic interactions. Here, we introduce a dual-atom Fe/Cu-NC catalyst synthesized through a metal–organic framework (MOF)-derived method where Fe and Cu atoms are uniformly dispersed on a porous nitrogen-doped carbon matrix, forming dual heteroactive Fe–N4 and Cu–N3 sites. The strategic combination of these active sites significantly enhances catalytic performance, achieving a 67.4% Faradaic efficiency (FE) for ethanol at −0.8 V vs RHE in CO2-saturated 0.5 M KHCO3. In situ spectroscopic analysis confirms the formation of major *CO and *CHO intermediates during CO2 electrolysis on the Fe/Cu-NC electrode, which are crucial for C–C coupling and ethanol production. DFT studies reveal that Fe–N4 and Cu–N3 sites synergistically lower the *CO intermediate energy barriers. Fe–N4 enriches the local CO concentration, which migrates to Cu–N3, enhancing ethanol production. This highlights MOF-derived dual-atom catalysts as a promising strategy for efficient CO2 conversion into ecofriendly products with zero emissions. |
| 關鍵字： | |
| 編號： | 4 |
| 期刊或研討會名稱： |
Applied Catalysis B: Environment and Energy
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| 著作名稱： | Cooperative dual single atom Ni/Cu catalyst for highly selective CO2-to-ethanol reduction
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| 年度： | 2024 |
| 類別： |
期刊論文
|
| 摘要： | |
| 關鍵字： | Atomically dispersed dual heteroactive sites Dynamic copper clusters Synergetic effect Accessible site populations CO2-to-liquid fuels |
| 編號： | 5 |
| 期刊或研討會名稱： |
International Journal of Hydrogen Energy
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| 著作名稱： | Atomically dispersed ruthenium single-atom alloy catalysts enabling efficient iodide oxidation reaction electrolysis in acidic media
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| 年度： | 2024 |
| 類別： |
期刊論文
|
| 摘要： | |
| 關鍵字： | Single-atom alloy Voltage efficiency Iodide oxidation Hydrogen evolution |
| 編號： | 1 |
| 期刊或研討會名稱： |
Chemical Engineering Journal
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| 著作名稱： | Novel electrocatalyst with abundant oxygen vacancies enabling efficient two-electron water oxidation reaction for H2O2 synthesis
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| 年度： | 2024 |
| 類別： |
期刊論文
|
| 摘要： | |
| 關鍵字： | Oxygen vacancy2e-WORNanomaterialElectrocatalystsH2O2Magnesium stannite tungstate |