ACS Catalysis
·
2024
·
IF 11.3
Longjian Li,Junhui Wang,Qinhua Zhang,Shuai Wang,Hangkai Zhang,Tao Xing,Mingqing Wang,Mingbo Wu,Zhenxing Wang,Wenting Wu
Near-infrared light occupies 54.3% of the solar spectrum and has greater penetration depth, and its effective utilization is of great significance in the practical application of photocatalysis on a larger scale. However, the development of catalysts that can directly utilize near-infrared light is still a huge challenge. This paper proposes a strategy to directly utilize near-infrared light (excitation wavelength extending to 850 nm) by creating carbon material doped with a high-spin-state Co(II)-Nx single-atom site. In the near-infrared-light-irradiated photooxidation of 1,5-dihydroxynaphthalene, the yield of juglone can reach 45% without a significant decrease, even when the catalytic volume is increased by 20 times, which was much higher than that irradiated by 460 nm wavelength (reduced by about 23%). Our study sets the stage for fabricating stable NIR photocatalysts and provides a solution to directly enhance NIR photooxidation in a large-scale manner.
研究领域:
材料科学
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光化学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
Advanced Energy Materials
·
2025
·
IF 26
Zongge Li,Wenjun Kang,Jingkai Lin,Rui Li,Konggang Qu,Suyuan Zeng,Lei Wang,Fanpeng Meng,Huayang Zhang,Haibo Li
The oxygen electrocatalytic activity of transition metal catalysts can be tuned by tailoring their microstructure to optimize electronic configuration. Here, a one-step Coordination-Selective Synthesis strategy is developed to integrate Co single-atom sites and Fe-based nanoparticles within the same matrix, enabling long-range electronic interactions that enhance Co-N 4 reactivity and improve oxygen reduction reaction performance. X-ray absorption spectroscopy confirmed that remote Fe-based nanoparticles modulate the electron distribution at Co-N 4 sites. Structural characterizations reveal that the optimal catalyst, Co 50% Fe 50% -NC, contains metallic Fe, Fe 3 O 4 , and Fe 4 N species. Electrochemical measurements show that it achieves onset and half-wave potentials of 0.984 and 0.927 V versus RHE, surpassing Co 100% -NC with only Co-N 4 sites. Additionally, it demonstrates efficient oxygen evolution reaction performance, achieving an overpotential of 298 mV at 20 mA cm −2 , comparable to RuO 2 . Density functional theory calculations reveal that Fe 4 N optimizes O-containing intermediate adsorption/desorption, lowering the theoretical overpotential. Zn-air batteries assembled with Co 50% Fe 50% -NC exhibited superior performance to Pt/C, highlighting its potential for bifunctional oxygen electrocatalysis. This study provides an approach for designing high-performance catalysts by utilizing synergistic interactions between atomic and nanoscale metal species.
研究领域:
材料科学
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电化学
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催化科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Meiling Fan,Peipei Liu,Yapeng Cheng,Haolin Tang,Bing Jin,Haining Zhang
Design and synthesis of earth-abundant elements-based electrocatalysts with sufficient activity and stability remain challenging for oxygen-involved electrochemical energy conversion and storage devices. In this work, catalyst with simultaneously engineered Fe-N 4 and Co-N 4 active sites and graphitic carbon multilayer-encapsulated FeCo alloy is developed by pyrolysis of metal salts doped G-g-C 3 N 4 . The obtained composite material exhibits promising catalytic activity and good stability for both oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) in alkaline electrolyte , as evidenced by the positive shift of half-wave potential by 44 mV compared to 20% Pt/C for ORR and the potential of 1.596 V at current density of 10 mAcm −2 for OER. In addition, the thus-assembled rechargeable zinc-air battery using the synthesized material as cathode delivers a maximum power density of 311.2 mWcm −2 with an open circuit potential of 1.51 V and a long-term cycling stability. DFT calculation results indicate that catalyst with composite active sites displays smaller energy barrier than that with single active site.
研究领域:
材料科学
·
电化学能源
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 23
·13678-13687
·
IF 12.732
Dan Wang,Hao Xu,Peixia Yang,Xiangyu Lu,Jingyuan Ma,Ruopeng Li,Lihui Xiao,Jinqiu Zhang,Maozhong An
Compared to individual metal sites, e.g. Fe–N4 sites, the synergistic effect of dual-metal sites can further adjust the interaction of reactants or intermediates with active sites, which is beneficial for boosting the oxygen reduction reaction (ORR) in Zn–air batteries. However, developing a simple and direct method instead of complicated procedures and post-treatment to realize well-defined dual-metal sites is still a grand challenge. Herein, a facile one-step impregnation-pyrolysis route without any post-treatment is developed to controllably synthesize Fe and Co dual-metal sites embedded in hierarchical N-doped carbon from metal–organic frameworks. X-ray absorption spectra coupled with density functional theory calculations demonstrate that the Fe–N4 and Co–N4 dual sites can synergistically enhance the ORR activity. Impressively, the well-controlled FeCo–N–C catalyst exhibits excellent ORR performance, with half-wave potentials (E1/2) of 0.807 and 0.904 V in 0.1 M HClO4 and 0.1 M KOH, respectively. Benefiting from the highly active dual-metal sites and desired porous structure, FeCo–N–C serving as a cathode catalyst achieves an uplifting peak power density of 196.3 mW cm−2 and a remarkable specific capacity of 728.6 mA h gZn−1 at a discharge current density of 20 mA cm−2 in a practical liquid Zn–air battery. Besides this, such superb battery performance is demonstrated in an all-solid-state Zn–air battery.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Huajie Zhong,Junhui Wang,Bin Zhang,Yangyang Liu,Zeyu Gong,Xinzhe Xiao,Jiaxing Yu,Yu Hou,Yuan Tao,Huangsheng Yang,Qi Fu,Jiating Zheng,Pengfei Wang,Gangfeng Ouyang
Carbon-supported single-atom catalysts (CS-SACs) have attracted tremendous attention in environmental remediation fields, however, the role of the ubiquitously existing carbon defects on the support in regulating the electronic structure of active metal sites has long been overlooked. Herein, a selective pyridinic N etching strategy is proposed to controllably fabricate specific pentagon defects in the carbon supports anchored with Co-N 4 sites. Theoretical and experimental results reveal that the pentagon defects can induce upward shifting of the Co d-band center and increase the electron density in the dxz and dz 2 orbitals, indicating its indispensable role in regulating the electronic structure of the metal center. As a result, efficient electron transfer is realized between the Co atom and peroxymonsulfate (PMS). Moreover, the energy barriers for crucial oxygen intermediate are reduced, which facilitates the generation of singlet oxygen ( 1 O 2 ). Consequently, the Co-N 4 catalyst with pentagon defects (C5-Co-N 4 ) achieved a remarkable TOF value (9.37 min −1 ) in a Fenton-like reaction, surpassing the state-of-the-art single-atom catalysts reported so far. This work not only provides a strategy to controllably fabricate specific defects in CS-SACs but also deepens the fundamental understanding on how pentagon defects regulate the electron structure and catalytic performance of metal-N 4 sites.
研究领域:
环境科学
·
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2020
·Vol. 8
·期 8
·4369-4375
·
IF 11.301
Lulu Chen,Yelong Zhang,Lile Dong,Wenxiu Yang,Xiangjian Liu,Ling Long,Changyu Liu,Shaojun Dong,Jianbo Jia
Rational design of isolated metal atom doped carbon catalysts is essential for revealing the essence of high activity for the oxygen reduction reaction (ORR), which can promote the development of robust catalysts for clean energy conversion devices. Herein, we report a simple one-step strategy to prepare Fe and Co atomically supported on N-doped nanocarbon (FeCo-IA/NC) from metal–organic frameworks with excellent ORR activity. The isolated Fe–N4 and Co–N4 sites are characterized by atomic-resolution aberration-corrected scanning transmission electron microscopy and X-ray absorption fine structure spectroscopy. The electrochemical results and density functional theory calculations indicate that the synergetic effect between Fe–N4 and Co–N4 accounts for the enhanced ORR activity. Benefiting from the large BET surface area, microporous feature, and high content (85%) of pyridinic and graphitic N, the well-designed catalyst exhibits better ORR activity (half-wave potential of 0.88 V) and Zn–air battery performances (higher open circuit potential and power density) than commercial Pt/C. This work may lay a foundation for further exploring efficient non-precious metal-based catalysts for the ORR and developing clean energy conversion devices.
研究领域:
材料科学
·
电化学
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Nano
·
2025
·
IF 16
Xiao Ge,Xinya Liu,Jinze Xu,Xiyang Zheng,Li-jiao Tian,Xiaozhi Wang
Rational regulation of the coordination environment of single-atom catalysts (SACs) is a promising yet challenging strategy to enhance their activity. Here, we introduce an O atom into the second coordination shell of Co–N4 sites via a simple thermal treatment, forming a Co–N4–ON matrix to boost photosynthetic hydrogen peroxide (H2O2) production. This modification significantly alters the electronic structure of the Co site, bringing the d-band center closer to the Fermi energy and elevating the conduction band of Co–N4–CN to enhance its reducing capacity. Density functional theory (DFT) calculations reveal intensified charge redistribution and a reduced work function in Co–N4–ON, facilitating O2 adsorption. Notably, Co–N4–ON exhibits the lowest O2 adsorption energy, indicating a stronger interaction between Co–N4–O and O2, which is further strengthened by orbital hybridization and charge transfer at their interface, leading to enhanced O2 activation. The optimized Co–N4–ON catalyst demonstrates superior O2 reduction capabilities with the lowest energy barrier during H2O2 desorption. Consequently, it achieves a H2O2 production rate of 3098.18 μmol g–1 h–1 under neutral conditions, which is 2.6 times higher than that of Co–N4–CN. Moreover, it maintains a production rate of 1967.79 μmol g–1 h–1 over 10 h in a continuous flow reactor under natural sunlight and ambient air, highlighting its durability and practicality. This study underscores the crucial role of the second coordination shell in SACs and offers valuable insights into their atomic-level structure–activity relationships, thus contributing to advancements in catalyst design for efficient photosynthetic H2O2 production.
研究领域:
化学
·
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Dan Xu,Ruirui Liu,Jianfeng Li,Huacheng Zhao,Jiantai Ma,Zhengping Dong
Transfer hydrogenation reactions using non-noble metal-based nanocatalysts are extensively attractive due to their low-cost and green reaction conditions. But construction of such catalysts with maximum metal atom efficiency and high catalytic activity is still a challenging research goal. Here, atomically dispersed Co catalysts with Co-N 4 active sites were fabricated, which builds a bridge for transfer hydrogenation between nitroarenes and saturated N-heterocycles in aqueous solution. The TOF value of the transfer hydrogenation reaction is much higher than nanoparticle catalyst for this reaction. Density functional theory (DFT) calculations and control experiments reveal that the excellent performance origins from the Co-N 4 sites, which combines the dehydrogenation of 1,2,3,4-tetrahydroquinoline with hydrogenation of nitrobenzene in one-pot. This work not only has an in-depth understanding of active sites but also shows a unique activity to the challenging, highly efficient, and green transfer hydrogenation reaction.
研究领域:
催化化学
·
材料科学
·
理论化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）