Journal of Bioresources and Bioproducts
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2026
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IF 19.9
Limin Zhou,Mengmeng Fan,Yanyan Liu,Shuling Liu,Guozheng Dong,Ao Wang,Jong-Min Lee,Kang Sun,Baojun Li
Single-atom catalysts (SACs) have advantages such as high atom utilization and well-defined active sites, and have been extensively studied in the field of oxygen electrocatalysis. However, current strategies for tuning the M-N 4 configurations predominantly focus on local coordination environments, which still makes it difficult to simultaneously optimize the balance of adsorption energies of oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) intermediates. Herein, a Zn volatilization-induced pyrolysis strategy is developed to construct Co-N 4 sites coupled with Co nanoparticles on curved N-doped biomass-derived carbon (Co NPs + SA @NC). The intrinsic curvature and defect-rich structure induce lattice distortion and electronic polarization, significantly enhancing the metal-support interaction (MSI). This curvature-enhanced MSI triggers electronic reconstruction and symmetry breaking of Co-N 4 sites, narrowing the highest occupied molecular orbital (HOMO)-lowest unoccupied molecular orbital (LUMO) gap and facilitating electron transfer. Meanwhile, the influence of adjacent Co nanoparticles optimizes the electronic structure of Co-N 4 , improving the adsorption-desorption capacity of intermediates in the OER process. Therefore, the half-wave potential required to achieve ORR was 0.87 V, and the overpotential required to reach a current density of 10 mA/cm 2 is only 290 mV. A zinc-air battery (ZAB) based on Co NPs + SA @NC exhibited a high peak power density of 172 mW/cm 2 . This work highlights curvature-mediated MSI as an effective strategy for controlling single-atom configurations and advancing biomass-derived electrocatalysts.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Ganghua Zhou,Longyun Zhang,Yu Xia,Hangmin Xu,Weiqin Yin,Shengsen Wang,Jianjian Yi,Xingwang Zhu,Xin Ning,Xiaozhi Wang
Solar-driven conversion of CO 2 into high-value-added chemicals is considered as one of the effective strategies to address global climate change. However, the sluggish charge separation kinetics and poor product selectivity remain the two major bottlenecks restricting photocatalytic CO 2 conversion. Herein, we developed an anatase surface modified atomically dispersed Cu (Cu anchored on N-doped carbon skeleton) photocatalyst (TiO 2 /Cu 1 NC) based on a “reflux + calcination” method for CO 2 photoreduction. Under full spectral illumination, the as-synthesized TiO 2 /Cu 1 NC displayed a brilliant CO production rate of 2.59 μmol h −1 (mass of photocatalyst: 5 mg), high selectivity (∼98.5%), and excellent durability using [Ru(bpy) 3 ]Cl 2 ·6H 2 O as the photosensitizer and triethanolamine as an electron donor. Experiments and density functionalized theory calculations synergistically confirm that the surface-constructed atomically dispersed Cu 1 NC active sites can accelerate the separation and transfer of photogenerated charge carriers, optimize CO 2 adsorption and activation, reduce the formation energy barrier of the key intermediate *COOH during the CO 2 RR process, and thus enhance the activity and selectivity of CO 2 RR. This work provides new insights into the surface engineering of atomically dispersed active sites to improve the activity and CO selectivity of CO 2 photoreduction.
研究领域:
材料科学
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环境科学
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Lingzhe Meng,Shuwen Niu,Zhengyu Wei,Xue Qin,Faheem Naseem,Wei Wei
Iron phthalocyanine (FePc) with tetracoordinated Fe-N 4 site shows promising activity for catalyzing the oxygen reduction reaction (ORR) in alkaline media. However, the consecutive proton-coupled electron transfer (PCET) steps with water as the proton donor and low electronic conductivity of FePc raise the kinetic barriers for device application. Herein, a significant effect of polyoxometalates (POMs) on the ORR kinetics of Fe-N 4 sites via surface coordination of FePc is revealed. POM clusters modulate the interactive steric/electronic environment of Fe-N 4 , leading to a low barrier for H 2 O cleavage to produce protons along with a high electron transfer rate, thereby accelerating the PCET steps of FePc. With precisely controlled electron charge of POM clusters, the influence and mechanism of heteropoly blue in promoting PCET steps of FePc relative to heteropoly acid are elucidated, and noticeably enhanced ORR activity and reaction current are achieved. These findings highlight the potential of POMs as ligands to optimize dynamics of Fe-N 4 atomic sites toward efficient alkaline ORR.
研究领域:
化学
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材料科学
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催化
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
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IF 22.1
Kui Wang,Bin Chen,Yimin Xuan,Wenjun Fan,Nan Sun,Sheng Chang,Guowen Meng
The CO 2 electroreduction (CO 2 RR) is extensively deemed as a promising route to reach carbon neutralization, while the single-atom catalysts (SACs) are proved to be effective in CO 2 RR. However, most SACs cannot further amplify performance due to their powdery feature. Herein, we present numerous isolated nickel single atoms anchored on 3D interconnected N-doped carbon tubes (NiSAs@3D-INCT) network as a self-supported electrode. The NiSAs@ 3D-INCT has truly interconnected and highly ordered vertical and lateral carbon tube-channels, which promote the CO 2 interaction and electrolyte transmission. The NiSAs@3D-INCT exhibits a superior CO 2 RR performance with an appreciable CO partial current density of 51.8 mA cm −2 at − 0.96 V versus the reversible hydrogen electrode (RHE). X-ray absorption fine structure spectroscopy and theoretical computations reveal the NiSAs are loaded on the 3D-INCT network with Ni-N 4 configuration as highly active sites for CO 2 RR. This work will shed a new light on opening up high performance SACs for CO 2 RR.
研究领域:
材料科学
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电化学
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催化科学
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高影响因子
Journal of Materials Chemistry A
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2024
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IF 10.7
Yuanzhe Zhao,Xiuheng Wang
Singlet oxygen (1O2) is an excellent active species for eliminating organic pollutants in single-atom catalyst (SAC) catalyzed peroxymonosulfate (PMS)-based Fenton-like systems. However, it is difficult to achieve high efficiency and selectivity in 1O2 generation as a result of the lack of effective SACs. In this work, a Co SAC (Co–N–C) containing highly uniform Co–N4 active sites with an ultralow-level Co loading of 0.34 wt% is fabricated, delivering boosted performance in tetracycline degradation with an extremely rapid rate of 0.573 min, which outperforms most advanced catalysts in reported studies. A vibrating-sample magnetometer is used to preliminarily determine the atomically dispersed Co sites in Co–N–C according to the obvious paramagnetic characteristics of Co–N–C, and this is in good agreement with the test results obtained by using an aberration-corrected high-angle annular dark-field scanning transmission electron microscope and synchrotron radiation facility. Electron spin resonance and free radical quenching experiments prove that Co–N–C facilitates PMS activation with the 1O2 generation of almost 100%. Mechanism analyses suggest that the Co–N4 site strengthens the adsorption of the terminal O of PMS, realizing enhanced electron transfer from Co–N–C to PMS, promoting the simultaneous and spontaneous cleavage of O–O and O–H bonds to produce O*, followed by a reaction with another O* to generate 1O2.
研究领域:
环境科学
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催化化学
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2022
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IF 6.76
Jingshun Shen,Qi Liu,Qiqi Sun,Jianwei Ren,Xue Liu,Zuoxu Xiao,Chuanwang Xing,Yuexing Zhang,Guangwu Yang,Yanli Chen
A novel two-dimensional (2D) single-atom Fe/N/C catalyst (Fe 1 Zn 30 NC PDI ) has been prepared upon pyrolyzing a well-designed quasi-Fe-/Zn-phthalocyanine-based polymer (qFePc 1 @qZnPc 30 @PDI). In the qFePc 1 @qZnPc 30 @PDI precursor, qFePc moieties containing Fe-N 4 sites are efficiently segregated by lots of qZnPc moieties connected together by perylene linkers, which not only leads to the larger specific area in the resulting Fe 1 Zn 30 NC PDI but more importantly ensures the in-situ formation of Fe-N 4 sites on the self-supporting 2D N-doped carbon backbone. Impressively, Fe 1 Zn 30 NC PDI exhibites its superior oxygen reduction reaction (ORR) electro-catalytic activity and peroxidase (POD)-like activity. For ORR in an alkaline medium, it exhibites a much higher onset potential of 0.97 V and half-wave potential of 0.89 V than 20 wt% Pt/C catalyst with good durability of 92 % retention rate after 20000 s. And, Fe 1 Zn 30 NC PDI also shows better peak power density (86 mW cm −2 ) compared with 20 wt% Pt/C in Zn-air battery. Benefiting from the specific POD-like activity of Fe-N 4 , the Fe 1 Zn 30 NC PDI also shows excellent and selective performance in colorimetric H 2 O 2 sensing, with the ultrafast response (30 s), a low limit of detection (10 nM), and good robustness. This work sheds light on a promising design concept for synthesizing 2D polymer-derived single-atom multifunctional catalysts.
研究领域:
材料科学
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电化学
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分析化学
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Mengxia Shen,Jiale Qi,Kun Gao,Chao Duan,Jun Liu,Qingqing Liu,Hao Yang,Yonghao Ni
Fe-N x C single-atom catalysts have been immensely explored as the most promising ORR catalysts for replacing noble metals. Nevertheless, how to precisely introduce Fe atoms to optimize their spatial distribution and coordination environment in carbonaceous matrices while constructing the hierarchical porous structures to facilitate the mass transport process and ensure the accessibility of Fe-N x sites remain significant challenges. Here, we propose a strategy to prepare porous N -doped carbon aerogels anchored with single atomic Fe sites (Fe-SA@PNC) as highly efficient ORR electrocatalysts via directional freeze-casting and chemical vapor deposition. Fe-SA@PNC exhibit remarkable ORR activity and stability due to the highly stable honeycomb morphology and hierarchical pore structure, as well as the atomically dispersed Fe-N 4 sites in the carbon support. Furthermore, the practical application of Fe-SA@PNC catalysts as cathode materials in Zn-air batteries was demonstrated with encouraging performance. This study provides a promising approach for constructing high-efficiency ORR single-atom catalysts.
研究领域:
材料科学
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电化学
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ACS Sensors
·
2026
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IF 10.9
Fan Shi,Shu Deng,Lianjin Jiang,Jidie Tao,Yongfa He,Jinju Zuo,Brij Mohan,Wei Sun,Qiantao Ma
Chlorogenic acid (CGA) has antibacterial, antiviral, and antioxidant properties, making its detection essential in food science, pharma, and environmental monitoring. Nevertheless, the mechanistic understanding of CGA recognition and redox behavior at electrochemical sensor interfaces remains limited, posing a key scientific challenge. Herein, a novel Fe-N4 diatomic-site carbon nanomaterial is prepared via in situ pyrolysis of coffee grounds, which served as a simultaneous precursor for carbon, iron, and nitrogen. Aberration-corrected scanning transmission electron microscopy confirms single-atom dispersed iron with diatomic active sites. At the same time, X-ray absorption near-edge structure and extended X-ray absorption fine structure analyses reveal a Fe–N4 coordination. Density functional theory calculations indicate that during CGA oxidation, hydroxyl oxygen atoms preferentially adopt a side-adsorption configuration at dual active sites, thereby enhancing interfacial electron transfer and catalytic selectivity. The constructed electrochemical sensor exhibits two linear response ranges, 0.2−0.8 and 0.8−500.0 μmol/L, with a detection limit of 0.067 μmol/L (LOD = 3 s/m). Overall, this study presents a sensitive, cost-effective electrochemical sensor for CGA detection and highlights the critical role of adsorption configuration in determining the performance of single-atom catalysts.
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高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2025
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IF 11.3
Shichao Cai,Yurou Tan,Hongyi Li,Liwei Yang,Bo Chen,Feng He
Zero-valent iron (ZVI, Fe0) can effectively reduce a variety of chlorinated hydrocarbons. However, ZVI is incapable of dechlorinating 1,2-dichloroethane (1,2-DCA), a commonly found contaminant in groundwater, and the existing ZVI modification methods have little effect on this predicament. In this study, we prepared ZVI composites modified with Fe–N4 coordination structure (Fe0@FeNC), which exhibited outstanding dechlorination performance toward 1,2-DCA. Fe0@FeNC (1 g/L) can degrade 94% of 1,2-DCA (10 mg/L) within 37 days, with an ethene selectivity of nearly 100%, whereas nanoscale ZVI (nZVI) or even Pd-doped nZVI and sulfidated ZVI cannot degrade 1,2-DCA. The results from X-ray diffraction patterns and Mössbauer spectra confirmed the presence of Fe0 and Fe–N4 coordination structure in the Fe0@FeNC, which were proven to be the electron donor and dechlorination active center for 1,2-DCA dechlorination, respectively. Theoretical calculation reveals that the Fe–N4 coordination structure can reduce the free energy required for 1,2-DCA reduction, thus allowing 1,2-DCA to utilize electrons provided by Fe0 to achieve dechlorination. These findings can guide the design of ZVI-based materials to achieve in situ abiotic remediation of 1,2-DCA-contaminated groundwater.
研究领域:
环境科学
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材料化学
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化学工程
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污染修复
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PubMed
高影响因子
Nano-Micro Letters
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2026
·Vol. 18
·期 1
·96
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IF 36.3
Fang Wenhan,Xu Kailong,Wang Xinlei,Zhu Yuanhang,Li Xiuting,Liu Hui,Li Danlei,Wu Jun
A universal synthetic strategy was proposed to construct heteroatom axially coordinated Fe–N 4 single-atom seawater catalyst materials (Cl–Fe–N 4 and S–Fe–N 4 ).
The Cl–Fe–N 4 catalyst achieves a limiting current density of 5.8 mA cm −2 and a half-wave potential of 0.931 V vs. RHE in alkaline synthetic seawater, outperforming commercial Pt/C (40 wt%).
The seawater-based zinc-air battery fabricated with Cl–Fe–N 4 demonstrates a power density of 187.7 mW cm −2 at 245.1 mA cm −2 and maintains stable cycling performance for 200 h.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Fantao Kong,Yifan Huang,Meixin Chen,Ge Meng,Han Tian,Yafeng Chen,Ziwei Chang,Chang Chen,Wenping Sun,Xiangzhi Cui,Jianlin Shi
The performance of oxygen reduction reaction (ORR) on Fe-N-C single-atom catalysts (SACs) is still less satisfactory due to the rather low atom-utilization of active sites. Here, a novel acetate thermolysis-assisted route is proposed to create hierarchical carbon nanocages of Fe-N-C SACs (Fe SA -N/Cs-OAc) by selective cleavage of carbon layers, which features abundant edge-sited Fe-N 4 moieties in well-defined mesoporous channels. Benefiting from the ultra-high site density and utilization of Fe-N 4 moieties, the optimized Fe SA -N/Cs-OAc catalyst demonstrates excellent ORR activities marked by extraordinarily high half-wave potentials ( E 1/2 ) of 0.94 V and 0.82 V in alkaline and acidic electrolytes. Zn-air battery using Fe SA -N/Cs-OAc as cathode delivers a power density of 165 mW cm −2 , and the maximum output power in H 2 -O 2 fuel cell reaches 640 mW cm −2 . The abundant mesoporosity makes most Fe-N 4 sites accessible and simultaneously produces in-plane pore defects that reduced adsorption energy of *OH (−0.72 eV), finally presenting remarkably enhanced ORR performance.
研究领域:
材料科学
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电化学
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催化科学
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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IF 9.9
Chao Chen,Shilong Zhou,Jiawei Xia,Le Li,Xingyue Qian,Fengxiang Yin,Guangyu He,Haiqun Chen
Exploring efficient, easy-to-manufacture, and inexpensive bifunctional electrocatalysts with abundant accessible active sites is crucial for rechargeable zinc-air batteries (ZABs). Herein, we report the strategy consisting of the space confinement and pore-making engineering to fabricate single-atom catalyst enriched with Fe-N 4 sites anchored on N -doped hierarchically porous carbon (Fe-NC-C 3 N 4 ). The optimized Fe-NC-C 3 N 4 exhibits excellent oxygen reduction/evolution reaction (ORR/OER) activities with a half-wave potential ( E 1/2 ) of 0.90 V vs. RHE and a promising low overpotential of 0.305 V vs . RHE at 10 mA·cm −2 in alkaline electrolyte. These superior catalytic activities are attributed to the combined effect between the atomic active sites and the well-balanced micro-meso-macropore structures. The homemade liquid Zn-air battery (ZAB) assembled with Fe-NC-C 3 N 4 catalyst displays a power density of 133.59 mW·cm −2 and a significant energy density of 882.58 mAh·g −1 , exceeding those of the equipment with commercial Pt/C-RuO 2 (56.82 mW·cm −2 and 643.87 mAh·g −1 , respectively). Particularly, the corresponding flexible wearable ZAB manifests outstanding foldability and cyclical stability. This work opens a new perspective for the structural design of single-atom catalysts in the energy storage and conversion area.
研究领域:
材料科学
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能源存储与转换
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PubMed
高影响因子
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