CHINESE JOURNAL OF CATALYSIS
·
2025
·
IF 17.7
Guohao Na,Hongshun Zheng,Mingpeng Chen,Huachuan Sun,Yuewen Wu,Dequan Li,Yun Chen,Boran Zhao,Bo Zhao,Tong Zhou,Tianwei He,Yuxiao Zhang,Jianhong Zhao,Yumin Zhang,Jin Zhang,Feng Liu,Hao Cui,Qingju Liu
Metal-support interaction (MSI) is regarded as an indispensable manner to stabilize active metals and modulate catalytic activity, which shows great potentials in developing of efficient hydrogen evolution reaction (HER) electrode with high activity and strong robustness. Herein, this work presents a novel heterostructure with ultrafine platinum quantum dots (Pt QDs) on defective catalytic supports derived from metal-organic frameworks (MOFs). It is indicated substantial oxygen vacancies can be generated and Pt–Pt bonds can be optimized through topological transformation. The resulting Pt/T-NiFe-BDC (BDC: C 8 H 6 O 4 ) exhibits competitive HER activity in alkaline seawater, attaining ultralow overpotentials of 158 and 266 mV at 500 and 1000 mA cm –2 with fast kinetics and outstanding stability. An asymmetric water electrolyzer using Pt/T-NiFe-BDC as a cathode only requires a voltage of 1.89 V to generate an industrial density of 1000 mA cm –2 and shows no attenuation in 500-h continuous test at 500 mA cm –2 . Theoretical calculations and in-situ spectroscopic analysis reveal the reversible hydrogen spillover mechanism, in which oxygen vacancies facilitate the sluggish water dissociation and Pt QDs promote the H* combination. This study provides a new paradigm to engineer metal-supported catalysts for efficient and robust seawater splitting.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2019
·
IF 7.723
Bo Ye,Ronghua Jiang,Zebin Yu,Yanping Hou,Jun Huang,Boge Zhang,Yiyi Huang,Yalan Zhang,Runzhi Zhang
The preparation of Pt quantum dots (Pt QDs) is an effective way that can solve the high cost problem by reducing the high dosage requirement of noble metal Pt. On the other hand, organic metal framework (MOF) can be used for the stabilization of metal nanoparticles with small size and uniform dispersion. Herein, we successfully synthesized a bifunctional electrocatalyst via a facile one-step hydrothermal treatment. Pt QDs cores are uniformly coated with Fe-MOF nanosheet arrays shell (Pt QDs @Fe-MOF) with a porous cuboids structure on Ni foam (NF). With the quantum size and core-shell structure, the self-assembled porous cuboids of Pt QDs @Fe-MOF exhibited perfect electrochemical performance for hydrogen evolution reaction (HER), oxygen evolution reaction (OER) and overall water splitting. Particularly, the electrocatalyst with ultralow content of Pt QDs (1.84 μg cm −2 ) only needed the overpotential of 33 mV and 191 mV to achieve 10 and 100 mA cm −2 in 1 M KOH, respectively. In addition, the Pt QDs @Fe-MOF/NF electrodes possessed remarkable activity and stability to deliver a current density of 10 mA cm −2 at 1.47 V for overall water splitting of at least 100 h.
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
Advanced Science
·
2021
·Vol. 8
·期 22
·2102207
·
IF 16.806
Sin-Yi Pang,Weng-Fu Io,Jianhua Hao
Supported metallic nanoparticles render highly tunable physical and chemical properties to mixed-dimensionality materials in electrocatalysts. However, some supports are susceptible to being dissolved in acidic solution or are unstable in ambient air. The development of high-performance catalysts has been facing the major hurdles of the sluggish activity in alkaline solution and requesting high energy to stabilize the nanoparticles on their supports, challenging the pH-universality and the applicability of the supported metallic nanoparticles. Here, a one-step strategy is proposed to modulate the growth of Pt quantum dots (QDs) on HF-free MXene under atomic-level by a low-temperature metal–support interaction reaction. By controllable tailoring in the morphology and strain induced by terminations, Pt (111) QDs with a sub-nanoscale size of 1.15 nm are grown as 0D/1D heterostructure to overcome the restrictions of employing reduction gas and high annealing temperature. The catalyst exhibits a low overpotential of 33.3 mV for acidic solution, while 65.1 mV for alkaline solution at a specific current density of 10 mA cm −2 . This study not only paves a scalable pathway to developing cost-efficient catalysts in moderate conditions, but also demonstrates an effective surface modulation strategy for 0D/1D heterostructures.
研究领域:
材料科学
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电催化
·
纳米技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2024
·Vol. 34
·期 40
·2403863
·
IF 18.5
Huashuai Hu,Zhihang Xu,Zhaorui Zhang,Xiaohui Yan,Xiaoli Wang,Ye Zhu,Jiacheng Wang,Minghui Yang
Seawater hydrogen production, vital for sustainable energy solutions and freshwater preservation, faces challenges due to seawater complexity and high energy consumption. A strategy to modulate dehydrogenation kinetics of dual-phase metal nitrides using low-loaded Pt quantum dots (QDs), achieving stable and energy-efficient hydrogen generation is introduced. The Pt QDs@Ni 3 N-MoN/Ti catalyst displays outstanding bifunctional seawater catalytic performance, enabling efficient hydrogen production and hydrazine degradation in a flow anion exchange membrane water electrolysis (AEMWE) device. Operating at a low voltage of 1.41 V, it achieves 2 A cm −2 for 300 h, circumventing chlorine corrosion and yielding record-breaking energy equivalent input (2.68 kWh m −3 H 2 at 1 A cm −2 ), a 47.1% reduction compared to traditional methods. Integration with solar and biomass energy facilitates self-powered hybrid seawater hydrogen production, highlighting its potential applications. This work facilitates energy-efficient marine resource conversion to green hydrogen and offers viable insights into industrial hazardous pollutant degradation using metal-nitride electrocatalysts.
研究领域:
能源科学
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材料科学
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电化学工程
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2018
·
IF 4.439
Chao Ouyang,Yunxiang Chen,Ziyu Qin,Dawen Zeng,Jian Zhang,Hao Wang,Changsheng Xie
As a typical two-dimensional (2D) layered transition metal dichalcogenides (TMDs), tungsten disulfide (WS 2 ) has been considered as a promising sensing material for room-temperature NH 3 detection. However, the bulk WS 2 -based room-temperature NH 3 sensors can hardly recover to its initial state after turning off gas . Although the recovery rate of bulk WS 2 was accelerated by thinning method, the response of few- or monolayer WS 2 nanosheets (NSs) to NH 3 was sharply decreased. Here, in premise of keeping fast recovery rate, few- or monolayer WS 2 NSs modified with Pt quantum dots (QDs) were prepared for room-temperature NH 3 detection, which exhibited significantly enhanced sensing properties with fast recovery speeds. Especially, the response of nanocomposite to 250 ppm NH 3 is nearly 10 times than that of WS 2 NSs, which could be attributed to the significantly decreased initial conductivity caused by electrons flowing from higher Fermi level of Pt QDs to that of WS 2 NSs and the higher catalytic activity. Furthermore, the Pt S bonds confirmed by XPS results could benefit electrons transfer between the interface. We hope that the 0D/2D heterostructure system in this work could provide a direction to improve sensing properties of 2D TMDs-based room-temperature sensors.
研究领域:
材料科学
·
传感技术
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Lijun Liao,Zhenzi Li,Jing Lu,Yachao Xu,Wei Zhou,Ying Wu
Photocatalytic overall water splitting (POWS), a sustainable route for solar-to-hydrogen conversion, faces challenges from rapid charge recombination and material instability. This study demonstrates a 12-fold enhancement in POWS by integrating spin polarization through platinum quantum dots chemically bonded to brookite/anatase TiO 2 . Advanced characterizations, including X-ray absorption spectroscopy and X-ray photoelectron spectroscopy, confirm Pt-Ti coordination (with a bond length of 2.84 Å) and electron transfer to Pt, thereby enriching the active sites. Magnetic circular dichroism spectroscopy reveals spin-polarized band structures in Pt/TiO 2 , which are absent in pristine TiO 2 , thereby suppressing charge recombination. Under light irradiation, Pt/TiO 2 achieves H 2 and O 2 evolution rates of 310 and 150 µmol h −1 g −1 , respectively, and an apparent quantum yield of 2.1 % at 365 nm. Density functional theory calculations trace this enhancement to optimized hydrogen adsorption free energy and reduced oxygen evolution overpotential. Spin-polarized Ti 3d and Pt 5d orbitals near the Fermi level extend carrier lifetimes, while a shifted d-band center facilitates oxygen desorption. This work establishes spin polarization engineering via cocatalysts as a transformative strategy for POWS, introducing a spin-dependent mechanism that addresses intrinsic limitations in photocatalysis, and offers a pathway to efficient solar fuel generation.
研究领域:
光催化
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材料科学
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物理化学
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纳米技术
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能量转换
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固体物理
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表面科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）