JOURNAL OF CATALYSIS
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2021
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IF 7.92
Junhui Wang,Shimin Yin,Qinhua Zhang,Fengliang Cao,Yicheng Xing,Qingshan Zhao,Yang Wang,Wengang Xu,Wenting Wu,Mingbo Wu
Polymeric carbon nitride materials show intriguing prospects in numerous light-to-energy conversion applications, but seldom studies focus on their triplet energy transfer, leading to the insufficient lifetime for the photochemical process. Inspired by the porphyrin molecular photocatalyst, single-atom sites (Fe-N 4 ) as triplet sensitizing sites were fabricated in g-C 3 N 4 for the preparation of Fe-g-C 3 N 4 , which processes a long-lived triplet emissive state (τ PH = 4.93 μs). But under realistic condition for the large-scale production of catalyst, single atoms are inevitable to sinter, resulting in the formation of other metal species. Therefore, the photooxidation of 1,5-dihydroxynaphthalene (1,5-DHN) and the photocatalytic E-Z Isomerization of stilbene were selected as the model reactions to evaluate the influence of various Fe species on the triplet energy transfer. It was found that Fe-N 4 sites promote the triplet energy transfer process, while Fe nanoclusters (Fe 0 ) promote the electron transfer and inhibit triplet energy transfer. This finding provides guidance for the rational design of photocatalysts to efficiently improve triplet energy transfer process and its application.
研究领域:
材料科学
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光化学
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DOI
高影响因子
CARBON
·
2024
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IF 10.5
Yinghua Wang,Lingmin Wu,Konggang Qu,Xiujun Wang,Baitao Li
The oxygen reduction reaction (ORR) is a crucial step in the energy transformation devices, which requires the fabrication of a cost-effective and energy-efficient Fe single-atom catalyst (SAC) to substitute platinum. However, achieving a controllable synthesis of Fe SAC is a formidable challenge. In this study, a Fe SAC with a novel 3D-on-2D architecture was fabricated by coating 3D metal-organic frameworks (MOFs) over the surface of 2D reduced graphene oxide (rGO). In-situ combining MOF and rGO in a composite structure by adjusting their weight proportion is a key to preparing an active 3D-on-2D structured catalyst with FeN 4 active sites. Thanks to the favorable conductivity of the 2D rGO-derived carbon structure and the 3D MOF structure exposing an enhanced density of FeN 4 sites, FeNC@rGO-2 demonstrates exceptional ORR activity. It performs more effectively than commercial Pt/C, exhibiting excellent half-wave potentials of 0.887, 0.705, and 0.741 V in alkaline, neutral, and acidic solutions respectively. Impressively, FeNC@rGO-2 exhibits excellent stability and methanol tolerance. When FeNC@rGO-2 is assembled as cathode catalyst in Zinc-air batteries (ZAB) and microbial fuel cells (MFC), FeNC@rGO-2-ZAB reveals outstanding power density (393 mW cm −2 ) and good charge/discharge cycling stability. Amazingly, FeNC@rGO-2-MFC also shows superior power density (2810 ± 19 mW m −2 ) and efficiency of electron recovery. This study reveals that FeNC@rGO-2 has extremely high application value in energy conversion devices oriented for alkaline and neutral electrolytes.
研究领域:
材料科学
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电化学
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能源转换
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DOI
高影响因子
Scientific Reports
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2017
·Vol. 7
·期 1
·1-14
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IF 4.259
Wang Baochen,Liu Yan-gai,Huang Zhaohui,Fang Minghao,Wu Xiaowen
Discovery of novel phosphors is one of the main issues for improving the color rendering index (CRI) and correlated color temperature (CCT) of white light-emitting diodes (w-LEDs). This study mainly presents a systematic research on the synthesis, crystal structure variation and photoluminescence tuning of novel (oxy)nitride solid solution Ca 3 Si 3− x
O 3+ x
N 4−2 x
: Eu 2+ phosphors. XRD refinements show that lattice distortion occurs when x value diverges the optimum one ( x = 1). The lattice distortion causes a widening of emission spectrum and an increase of Stokes shift (ΔSS), which leads to a bigger thermal quenching. With decrease of x value, the emission spectrum shows an obvious red-shift from 505.2 to 540.8 nm, which is attributed to the crystal field splitting. The enhanced crystal field splitting also broadens the excitation spectrum, making it possible to serve as the phosphor for near ultraviolet (n-UV) LEDs. A 3-phosphor-conversion w-LED lamp was fabricated with the as-prepared phosphor, which exhibits high CRI (Ra = 85.29) and suitable CCT (4903.35 K). All these results indicate that the Ca 3 Si 3− x
O 3+ x
N 4−2 x
: Eu 2+ phosphor can serve as the green phosphor for n-UV w-LEDs, with a tunable spectrum by controlling the crystal structure and morphology.
研究领域:
材料科学
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光学工程
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DOI
高影响因子
RARE METALS
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2025
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IF 11
Zhi Song-Song,Zou Xiao-Xiao,Lei Jin-Ye,Zhang Lu,Li Zi-Han,Gu Wan-Nuo,Ullah Fahim,Guo Hong,Wu Da-Peng
Photocatalytic CO 2 reduction using atomically dispersed catalysts holds significant potential for addressing global energy and environmental challenges. However, the influence of d–d orbital interactions between metal centers and coordinated atoms remains underexplored. Herein, nickel phthalocyanine is anchored to the metal-exposed crystal face of TiO 2 , forming Ti–Ni–N 4 coordination. This configuration reveals that the axially coordinated Ti atoms serve as a novel electron channel with electron-donating ability, transferring electrons to the Ni center through d–d coupling. It is found that the dynamic adjustment of bond lengths and d-band centers in Ti–Ni bonding during CO 2 photoreduction process can effectively modulate the adsorption strengths of the Ni center for different intermediates. This leads to a significant enhancement in the photocatalytic performance for CO 2 reduction to CO without a sacrificial reagent, achieving an exceptional CO evolution rate of 378.5 μmol g −1 . Furthermore, the d–d coupling mediated by Ti–Ni–N 4 coordination increases the vacancy formation energy of active sites, preventing the leaching of Ni active centers. This study provides a strategy for the precise design of d–d orbital regulation and resistance to demetallization in photocatalysts for efficient CO 2 conversion. Graphic abstract
研究领域:
催化
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材料科学
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环境科学
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无机化学
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光物理
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DOI
高影响因子
AICHE JOURNAL
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2025
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IF 4
Hai Zhang,Yixuan Meng,Fan Wang,Ze Zhang,Zhenyu Yang
This work introduces nickel (II) tetraphenylporphyrin (NiTPP) as a multifunctional electrolyte additive to simultaneously address polysulfide shuttle and uncontrolled lithium dendrite growth in lithium–sulfur (Li–S) batteries. Mobile NiTPP species act as homogeneous catalysts with Ni–N 4 centers for rapid polysulfide redox mediation to suppress migration, while planar molecules featuring lithium-affinity capability migrate to the lithium metal surfaces, enabling uniform lithium flux and anode protection. NiTPP-modified electrolytes significantly enhance Li–S battery performance, demonstrated by 634.9 mAh g −1 at 4C, 758.3 mAh g −1 after 100 cycles at 0.2 C (83.4% retention), and 757.5 mAh g −1 under high sulfur loading (2.9 mg cm −2 ) with lean electrolyte ( E / S = 5 μL mg −1 ), all with high Coulombic efficiency. Crucially, NiTPP, acting as a soluble dual-functional mediator enabling homogeneous operation in electrolytes, simplifies Li–S battery fabrication while demonstrating the commercial viability of molecularly engineered mobile active sites for stabilizing both electrodes in high-energy-density Li–S batteries.
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高影响因子
ACS Applied Polymer Materials
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2025
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IF 4.7
Tianping Wang,Yining Liang,Jingle Wang,Xikui Liu,De Ning,Zhengjian Chen
Covalent organic polymers have emerged as promising platforms with tailorable structures for electrocatalytic oxygen reduction reaction (ORR). However, their catalytic activities are often limited by dense stacking and low conductivities. Herein, we report an arylamine-linked iron-phthalocyanine (AAm-FePc) in situ grown on Ketjenblack (KB) (AAm-FePc/KB) via a condensation reaction between 2,9,16,23-tetraaminophthalocyaninato iron and dimethyl succinyl succinate. Characterizations reveal that AAm-FePc is uniformly distributed on the surface of KB, which provides a large accessible surface area and efficient electrical conductivity. Owing to abundant arylamine linkages present in the skeletons and precisely designed highly active Fe–N4 sites, the AAm-FePc/KB catalyst exhibits excellent ORR characteristics in alkaline media, including a half-wave potential of 0.883 V, fast kinetics (Tafel slope = 33 mV dec–1), a nearly four-electron reduction pathway and excellent methanol resistance and electrochemical stability. The AAm-FePc/KB-catalyzed Zn–air battery exhibits a high power density (177.8 mW cm–2), a large specific capacity (727 mAh g–1), and outstanding cycling stability (375 cycles, 125 h), which are superior to those of commercial Pt/C catalyst.
研究领域:
材料科学
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电化学
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催化
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能量存储与转换
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聚合物化学
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高影响因子
BMC MICROBIOLOGY
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2025
·Vol. 26
·期 1
·189
·
IF 4.2
Tian Shen,Deng Jiaxin,Kuang Dai,lv Meiping,Zhu Qiao,Zhang Nan,Liu Wei,Yi Jiling,Xia Qianfeng,Wang Yanshuang
Background Melioidosis, caused by Burkholderia pseudomallei , is a tropical disease that poses a serious risk of fatal sepsis and imposes a substantial financial burden on healthcare systems, driven by its complicated antibiotic resistance profile. With the successful isolation of vB_BpP_HN01 in Hainan, a theoretical basis for phage therapy has been established. Whilst the observation of certain clinical isolates non-susceptible to its infection, along with concerns about the potential emergence of tolerance during monophage treatment, highlights the urgent need to develop a broader and more diverse phage arsenal. Methods Phage screening was performed on environmental samples collected at sites geographically distinct from the original isolation location via B. pseudomallei HNBP001, a Hainan representative strain previously employed as the isolation host. Candidates characterized by host range and plaque properties were subjected to assays assessing environmental stability, infection and proliferation traits. Genetic features were analyzed by sequencing and comparative bioinformatics, followed by efficacy evaluation in A549 cell infection assays and Galleria mellonella larvae. Statistical analyses included one-way ANOVA and Kaplan–Meier survival curves with log-rank tests. Results A total of four podoviruses (vB_BpP_HN02 – HN05), with highly efficient (≥ 92%) and complementary lytic activities, were recovered from natural sources in Wenchang and Qiongzhong. Each exhibited distinct plaque morphology and robust viability, although compromised by exposure to high temperatures (≥ 60 °C) or extremely acidic conditions (pH ≤ 3). Highest titer production was demonstrated in vB_BpP_HN02 and vB_BpP_HN05 (2.5 × 10¹⁰ and 1.0 × 10¹¹ PFU/mL at optimal multiplicities of infection of 0.1 and 1, respectively), whilst complete bacterial clearance was achieved by the former. Genomic analysis classified them into the Schitoviridae family, sharing conserved N4-like architecture. Phage treatments restored the viability of infected A549 cells from 29.29% to 60.07–75.81%, with vB_BpP_HN02 displaying superior bactericidal capacity, even against the ceftazidime-resistant strain, further supported in the G. mellonella model, albeit modestly under single-dose administration. Conclusions As a continuation of our previous work, the identification of these phages addresses the natural occurrence of vB_BpP_HN01-insensitive strains and enhances understanding of B. pseudomallei phage diversity in Hainan. However, owing to close genetic similarity, cocktail formulation remains unfeasible, warranting further efforts to isolate more diverse novel phages.
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2026
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IF 19.7
Kaige Li,Jianhua Qu,Zhengni Pan,Yuxin Hou,Wenzhen Li,Mingyao Ma,Jingyi Wang,Juncheng Wang,Chengjun Ge,Jiwei Luo,Ying Zhang
Near-100% selective 1 O 2 generation via Fe-pyridinic N 4 sites. • Metal-atom utilization enhanced by 10 2 -10 4 -fold in FeSA-N-C-2S. • Fe-pyridinic N 4 shifts d -band center, lowering 1 O 2 energy barrier and tuning pathway. • 1 O 2 steady-state concentration positively correlates with Fe-pyridinic N 4 proportion. • A universal strategy creates various metal-based SACs with > 90% 1 O 2 selectivity. The type and quantity of nitrogen ligands in the first-shell coordination structure (FSCS) of single-atom catalysts (SACs) govern catalytic performance. However, current research largely focuses on nitrogen atom count, overlooking its chemical structure. Herein, by reconfiguring the FSCS from Fe-pyrrolic N 4 to Fe-pyridinic N 4 (FeSA-N-C-2S), we achieve selectivity approaching 100% for singlet oxygen ( 1 O 2 ) generation. Mechanistically, Fe-pyridinic N 4 shifts the d -band center toward the Fermi level via axial d_z² orbital hybridization, reducing Fe d -orbital occupancy, which enhances electron transfer through the conjugated π-system of pyridinic N, lowering the activation barrier for 1 O 2 generation and optimizing the reaction pathway. This facilitates complete degradation of electron-rich pollutants like 2,4,6-trichlorophenol, with a 4.3-fold increase in rate constant and a 21.5-fold higher metal-atom utilization efficiency compared to the FeSA-N-C-1S. Moreover, 1 O 2 steady-state concentration exhibits a significant linear positive correlation with Fe-pyridinic N 4 proportion, which can be precisely modulated by adjusting the pyrolysis temperature and metal-to-precursor ratio. This insight extends to other transition metals (Co, Cu, Mn), affording > 90% 1 O 2 selectivity. Long-term continuous-flow experiments and life-cycle assessments highlight the potential for scalable water treatment. Our work deciphers how coordination structure governs reactive oxygen species, providing a universal design paradigm for metal-pyridinic N 4 catalysts. Download: Download high-res image (210KB) Download: Download full-size image
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高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2022
·
IF 11.357
Mengxue Yang,Zexi Hou,Xin Zhang,Baoyu Gao,Yanwei Li,Yanan Shang,Qinyan Yue,Xiaoguang Duan,Xing Xu
Single-atom catalysts (SACs)-based peroxymonosulfate (PMS) systems are highly selective to the type of organic pollutants while the mechanisms remain ambiguous. In this work, we carried out experimental and theoretical investigations to reveal the origins of selectivity of radical and nonradical pathways in a designated Co–N4–C/PMS system. Two typical pollutants [bisphenol A (BPA) and metronidazole (MNZ)] with different molecular structures were employed for comparison. We found that radical oxidation (SO4•– and HO•) and nonradical electron-transfer pathway (ETP) co-existed in the Co–N4–C/PMS system. Pollutants (e.g., MNZ) with a high redox potential were degraded primarily by free radicals rather than ETP, while the oxidization of low-redox pollutants (e.g., BPA) was dominated by ETP at the surface region of Co–N4–C which overwhelmed the contributions of radicals in the homogeneous phase. Intriguingly, the contributions of radical and nonradical pathways could be manipulated by the PMS loading, which simultaneously increased the radical population and elevated the oxidation potential of Co–N4–C-PMS* complexes in ETP. Findings from this work will unravel the mysterious selective behavior of the SACs/PMS systems in the oxidation of different micropollutants.
研究领域:
环境科学
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催化化学
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DOI
高影响因子
Nature Catalysis
·
2025
·
IF 44.6
Zhao Kuang-Min,Wu Dao-Xiong,Wu Wen-Kun,Nie Jia-Bao,Geng Fu-Shan,Li Guang,Shi Hai-Yan,Huang Sheng-Chao,Huang Huan,Zhang Jing,Zhou Zhi-You,Wang Yu-Cheng,Sun Shi-Gang
Fe–N–C catalysts are the most promising alternative to Pt for the acidic oxygen reduction reaction (ORR), yet the electronic structure of their active centres remains elusive. Here we synthesize and characterize a conjugate-bridged iron phthalocyanine (FePc) dimer model catalyst with identical Fe sites and catalytic activity comparable to actual catalysts. A high-spin trivalent FeN 4 with an axial hydroxyl ligand, denoted as OH–Fe 3+ N 4 ( S = 5/2), is identified as the active state. By contrast, monomer and non-conjugated dimer manifest the OH–Fe 3+ N 4 ( S = 3/2) state with an excessive adsorption energy of ORR intermediates. Polymerized FePc is composed of 35% of the S = 5/2 state and 65% of the Fe 2+ N 4 ( S = 0 or 1) state, showing a general weaker adsorption energy. Both overly strong and weak adsorption energy hinder the ORR. Theoretical calculations indicate that π– d interaction between Fe and the conjugated carbon plane dictates the spin state. This study will help to precisely design Fe-based ORR catalysts.
研究领域:
材料科学
·
化学催化
·
电化学
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产品关联
DOI
高影响因子
Journal of Energy Chemistry
·
2020
·
IF 7.216
Xiaojing Jiang,Jianian Chen,Fenglei Lyu,Chen Cheng,Qixuan Zhong,Xuchun Wang,Ayaz Mahsud,Liang Zhang,Qiao Zhang
Controllable fabrication of Fe-N-C based single-atom catalysts (SACs) for enhanced electrocatalytic performance is highly desirable but still challenging. Here, an in situ surface-confined strategy was demonstrated for the synthesis of single atomic Fe-N 4 on N-doped carbon nanoleaves (L-FeNC). The in situ generated Zn 3 [Fe(CN) 6 ] 2 could not only serve as a protection layer against collapse of nanoleaves but also provide abundant Fe source for the formation of Fe-N moieties during pyrolysis, leading to high surface area and high graphitization degree of L-FeNC simultaneously. Benefiting from abundant Fe-N 4 active sites, enhanced mass and charge transfer, the as-prepared L-FeNC manifested a half-wave potential of 0.89 V for oxygen reduction reaction (ORR) in 0.1 M KOH. A maximum power density of 140 mW cm −2 and stable discharge voltage even after operation for 50,000 s have been demonstrated when the L-FeNC was used as air cathode for Zn-air battery. This work not only provided a unique surface-confined strategy for the synthesis of two-dimensional nanocarbons, but also demonstrated the significant benefit from rational design and engineering of Fe-N-C SACs, thus offering great opportunities for fabrication of efficient energy conversion and storage devices.
研究领域:
材料科学
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电化学
·
能源存储与转换
·
纳米科技
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催化化学
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DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2026
·
IF 11.3
Wei Wen,Chunying Wang,Xudong Chen,Jingyi Wang,Fei Wang,Kai Li,Yan Zhang,Yaobin Li,Changbin Zhang,Wenpo Shan
The development of high-efficiency non-noble-metal catalysts for HCHO removal is of great significance in indoor air purification. Zeolitic imidazolate frameworks (ZIFs) are characterized by large specific surface areas, well-defined porous structures, and tunable electronic properties, making them suitable for constructing single-atom catalysts with adjustable coordination environments. In this study, three Co-ZIF materials with distinct morphologies were synthesized and subsequently pyrolyzed, yielding cobalt-based catalysts with varied coordination structures. Among these catalysts, the Co–N–C(F) primarily features atomically dispersed Co species coordinated with four N atoms, forming Co-N4 active sites. Theoretical calculations indicate that the Co-N4 coordination structure exhibits enhanced oxygen activation compared to metallic cobalt sites, which is crucial for the degradation of intermediate products in the oxidation of HCHO. The Co–N–C (F) catalyst demonstrates superior activity in HCHO oxidation to even most noble metal catalysts. During a 710 h continuous test at 15 °C, the catalyst maintained 100% HCHO removal efficiency without observable deactivation. Simulation experiments further confirmed its practical applicability, with the catalyst module able to degrade 1 ppm of HCHO to <0.07 ppm within 2 h at room temperature. This work provides valuable insights for the development of commercial nonprecious metal catalysts for HCHO oxidation.
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DOI
PubMed
高影响因子
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