ACS Applied Energy Materials
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2022
·
IF 6.959
Xusheng Dong,Ruizheng Zhao,Haoxiang Di,Boya Wang,Guangzhen Zhao,Tingting Gao,Huapeng Li,Bin Sun,Dongliang Chao,Guowei Zhou
Carbonaceous materials are promising potassium-ion battery (PIB) anodes because of their merits of low cost and potentially porous structure. Unfortunately, sluggish kinetics of carbonaceous materials with limited active sites result in unsatisfactory cycling stability and poor rate performance. Herein, high active nitrogen sites are regulated through the additional phosphorus doping in 2D nitrogen-rich porous ultrathin carbon scrolls (P-N/UCS), realizing stable and high-rate potassium storage. Moreover, the P-N/UCS anode affords expanded interlayer distance and enhanced conductive networks with abundant pore structures and defects, which further accelerate charge transfer and K+ diffusion kinetics. Meanwhile, the P-N/UCS anode reveals a large specific surface area and high active N sites, which can expose additional open active sites to boost interfacial K+ adsorption reactions. Theoretical calculations further certify that the P-N/UCS anode can effectively enhance the adsorption capability of K+; thus, potassium storage performance is promoted. As a proof of concept, the as-prepared P-N/UCS anode exhibits a high specific capacity of 382.8 mAh g–1 after 500 cycles at 0.1 A g–1 and long cycle stability of 265.8 mAh g–1 after 2000 cycles at 1.0 A g–1. This work paves an avenue for the further controllable large-scale exploration of high-performance potassium storage anodes.
研究领域:
材料科学
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能源存储
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
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2023
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IF 9.5
Yuying Zhao,Qixin Yuan,Kang Sun,Ao Wang,Ruting Xu,Jing Xu,Yan Wang,Mengmeng Fan,Jianchun Jiang
Carbon material is considered a promising electrocatalyst for the CO2 reduction reaction (CO2RR); especially, N-doped carbon material shows high CO Faradic efficiency (FECO) when using pyridinic N species as the active site. However, in the past decade, more efforts were focused on the preparation of various carbon nanostructures containing abundant pyridinic N species and few researchers studied the electronic structure modulation of the pyridinic N site. The curvature of the carbon substrate is an easily controllable parameter for modulating the local electronic environment of catalytic sites. In this research, carbon nanotubes (CNTs) with different diameters are applied to modulate the electronic environment of pyridinic N by the curvature effect. The pyridinic N sites doped on CNTs with the average curvature of 0.04 show almost 100% FECO at the current density of 3 mA cm–2 at −0.6 V vs RHE and 91% FECO retention after 12 h test, which is superior to most of the carbon-based electrocatalysts. As demonstrated by density functional theory simulation, the pyridinic N site forms a strong local electric field around the nearby C active site and protrudes out of the curved CNT surface like a tip, which remarkably enriches the protons around the adsorbed CO2 molecule.
研究领域:
材料科学
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电化学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Shixuan Zhu,Dexu Zhang,Zhihong Xue,Yiqiang He,Cailing Chen,Zhan Shi
Establishing robust atomic-level interfaces, particularly through the selective modulation of surface active sites within heterojunctions to achieve superior solar energy conversion, remains largely unexplored. Herein, sulfur vacancy sites (V S ) in ZnIn 2 S 4 (ZIS) are selected, driven by the interaction between unsaturated zinc sites and the nitrogen-rich sites of g-C 3 N 4 , forming a step-scheme (S-scheme) heterojunction. The defect-induced interfacial Zn–N–C bonds not only provide rapid channels at the atomic level, thereby lowering the energy barrier for charge transfer, but also selectively tune the highly active pyrrolic N site to enhance H 2 evolution. Furthermore, molecular dynamics simulations (MD) combined with density functional theory (DFT) calculations reveal that V S regulates the pyrrolic N sites within the heterojunction, leading to a reduction in the Gibbs free energy for hydrogen production. Kinetic analysis by carrier transport activation energy (CTAE) indicates that the charge transfer energy barrier is accelerated, decreasing from 211.20 eV for ZIS/CN-360 % to 155.71 eV for V S -ZIS/CN-360 %. Consequently, the designed catalyst significantly enhances the H 2 yield (27.94 mmol g −1 h −1 ) in the absence of platinum. This work emphasizes the importance of generating defect-induced interfacial atomic channels, as well as changes in the surface microenvironment, which underscore the significance of defect heterostructures in promoting the photocatalytic process.
研究领域:
材料科学
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催化化学
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能源科学
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产品关联
DOI
PubMed
高影响因子
Nature Communications
·
2021
·Vol. 12
·期 1
·1-12
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IF 14.919
Xie Chao,Lin Longfei,Huang Liang,Wang Zixin,Jiang Zhiwei,Zhang Zehui,Han Buxing
Selective cleavage of C-C bonds is very important in organic chemistry, but remains challenging because of their inert chemical nature. Herein, we report that Zn/NC-X catalysts, in which Zn 2+ coordinate with N species on microporous N-doped carbon (NC) and X denotes the pyrolysis temperature, can effectively catalyze aerobic oxidative cleavage of C(CO)-C bonds and quantitatively convert acetophenone to methyl benzoate with a yield of 99% at 100 °C. The Zn/NC-950 can be applied for a wide scope of acetophenone derivatives as well as more challenging alkyl ketones. Detail mechanistic investigations reveal that the catalytic performance of Zn/NC-950 can be attributed to the coordination between Zn 2+ and N species to change the electronic state of the metal, synergetic effect of the Zn single sites with their surrounding N atoms, as well as the microporous structure with the high surface area and structural defects of the NC.
研究领域:
有机化学
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催化材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF POWER SOURCES
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2021
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IF 9.127
Li Zhong,Qi Huang,Junyang Ding,Yuanyuan Guo,Xian Wang,Lulu Chai,Ting-Ting Li,Yue Hu,Jinjie Qian,Shaoming Huang
It is of great importance to find non-precious metal based oxygen reduction reaction (ORR) catalysts with high stability, high performance and low cost. In this context, hierarchically porous carbon-based nanomaterials doped with heteroatoms are regarded as one of promising catalysts for ORR. Herein, a bottom-up approach is proposed by using the initial MOF-derived CoO@ZIF-67 core-shell structure as a template to obtain hollow cobalt-anchored N-doped carbon material followed by acid etching ( A-CoNC ). It exhibits a type of hollow porous nitrogen-carbon network anchored by well-dispersed atomic Co-N x sites with high activity and stable catalytic performance. The as-obtained A-CoNC shows high electrocatalytic ORR activity, good reaction selectivity with the low Tafel slope of 55.5 mV dec −1 , large limited current density of 5.37 mA cm −2 and excellent long-term stability (retention = 96.1%, time = 10 h). Furthermore, A-CoNC can also be serving as efficient electrocatalysts for zinc-air battery with a high power density of 144.0 mW cm −2 . Our synthetic strategy from the MOF-derived core-shell structure to ORR electrocatalyst provides new pathway for the design and preparation of highly efficient electro-/photo-catalysts stemmed from MOFs materials.
研究领域:
材料科学
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化学工程
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能源科学
✓ 已验证
产品关联
DOI
高影响因子
Energy Technology
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2022
·Vol. 10
·期 11
·2200602
·
IF 4.149
Xiaoran Zhu,Jianze Zhang,Yan Wang,Mingsheng Yang,Haiping Yu,Tengfei Li,Mingjun Hu,Jun Yang
It remains a challenge to achieve high-performance, low-cost, and robustly durable Fe, N co-doped carbon-based oxygen reduction reaction (ORR) catalysts with abundantly accessible Fe–N X sites. Herein, a novel scheme is designed to enrich the pore structure, increase the specific surface area, and generate spatially isolated Fe–N X sites of the ORR catalyst, in which pyridine nitrogen-rich lamellar metal–organic complex (Fe–tetrapyridophenazine) is employed as the precursor and 2D graphitic carbon nitride (g-C 3 N 4 ) as additional nitrogen source for achieving synergistic nitrogen-doping effect. The introduction of g-C 3 N 4 not only ameliorates the nitrogen coordination environment of metal active centers of the composite, but also increases the specific surface area and improves the pore structure. The resultant Fe–NC&CN composite has abundant active sites as well as remarkable electrical conductivity and suitable pore size for electron transfer and reactant diffusion. As expected, the catalyst exhibits excellent ORR activity, driving the reaction with low overpotential ( E 1/2 = 0.879 V) and remaining stable over a long reaction time (93% for 60 000 s), better than commercial Pt/C (20%) in all aspects. The assembled Zn–air battery exhibits high open-circuit voltage of 1.566 V and high specific capacity of 815 mAh g Zn −1 , as well as stable and persistent discharge performance.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
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2023
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IF 6
Yi Zhang,Donghao Liu,Weidong Guo,Yigang Ding
The development of stable and inexpensive adsorbents for La(III) recovery from wastewater is of great importance for rare earth industries. In this work, two novel N -rich covalent organic frameworks (COFs) synthesized via a one-step solvothermal method were termed as COF-PA-CC and COF-ML-CC, and employed as the adsorbents for removal of rare earth (RE) ions from aqueous solution. The structures and properties of COFs were characterized with X-ray diffractometer, total reflection infrared spectrometer, field-emission scanning electron microscopy, X-ray photoelectron spectroscopy, nitrogen adsorption–desorption instrument and thermogravimetric analyzer. The results revealed that COF-PA-CC composed of nanowires with the average length of 500 nm, whereas COF-ML-CC displayed the spherical morphology with the diameter of 100 ∼ 300 nm. Specific surface areas of COF-PA-CC and COF-ML-CC were calculated to be 82.13 and 191.08 m 2 /g, respectively. The adsorption process of La(III) was well-fitted with pseudo-second-order kinetic model and Langmuir isotherm model, exhibiting the high adsorption capacities of 150.88 and 168.19 mg/g for COF-PA-CC and COF-ML-CC after 120 min. Moreover, the influences of pH, temperature, different RE ions on adsorption performances were comprehensively tested, yielding an optimal adsorption condition (pH = 5.5, 65 °C and 120 min) and a better affinity for some light RE ions. Importantly, the fabricated COFs possess the excellent reusability after five adsorption-regeneration cycles, remaining 97.84 % and 95.51 % of initial capacities for COF-PA-CC and COF-ML-CC, respectively. The adsorption mechanism revealed that the complexation interaction between La(III) and the unoccupied N sites of N -rich COFs was recommended to interpret the remarkable adsorption performance of La(III) on the basis of the characterization analysis after the adsorption with elemental mapping, EDS and XPS. Consequently, these low-cost and robust COFs with abundant active N sites supplied a promising strategy for the recovery of RE ions from wastewater.
研究领域:
材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
INORGANIC CHEMISTRY
·
2025
·
IF 4.7
Ruiting Wang,Min Tian,Guanying Ye,Xinrui Li,Guoda Li,Suqin Liu,Zhen He
Metal-nitrogen (M-Nx) moieties are recognized as the most active sites in metal-nitrogen codoped carbon catalysts (M-N/C) toward the oxygen reduction reaction (ORR). Controllable construction of the M-Nx sites and effective exposure of them at the catalyst–electrolyte interfaces are critical for the high-efficiency electrocatalysis of oxygen reduction. Herein, a universal synthesis strategy is developed to construct surface-enriched and highly dispersed M-Nx sites of various metal centers (including Co, Fe, Cu, Ni, Mn, and Bi) in M-N/C by utilizing a prefabricated pyridine-nitrogen-rich carbon matrix to anchor the metal ions from the corresponding metal chloride vapors. All the as-synthesized M-N/C catalysts demonstrate outstanding ORR activities and excellent long-term stability, among which the optimized Co-N/C exhibits an exceptional ORR half-wave potential (E1/2) of 0.900 V vs RHE (VRHE) and only 6% current loss after testing at 0.60 VRHE for 16 h in a 0.1 mol L–1 KOH solution. This work opens new possibilities for the fabrication of high-performance M-N/C catalysts with various metallic centers or even multiple kinds of metallic centers for different applications.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Sustainable Chemistry & Engineering
·
2017
·
IF 5.951
Jiaoxing Xu,Chuxin Wu,Qiangmin Yu,Yi Zhao,Xun Li,Lunhui Guan
The utilization of metal and nitrogen doped carbon as a Pt-free oxygen reduction electrocatalyst depends largely on the homogeneous composition of the metal–nitrogen sites with limited content. Herein a simple and feasible ammonia defective activation strategy is explored on ordered mesoporous carbon (APC) to confine hematin precursor and suppress the formation of inorganic Fe-based derivatives during pyrolysis. Thus, a hierarchically nanoporous Fe/N/APC catalyst with high numbers of exposed iron–nitrogen sites exhibits an impressive performance for oxygen reduction reaction in alkaline media, with large diffusion-limited current density and positive half-wave potential with respect to commercial Pt/C catalyst. The enhanced ORR properties can be majorly ascribed to synergistic contributions of high numbers of exposed catalytic sites completion from high contents of Fe–N and pyridinic N along with the fast mass-transport properties arising from the etched high permeable porous structure. When applied as cathodic catalyst in Zn-air battery, it demonstrates a power density of 200 mW cm–2 and a specific capacity of 605 mA h g–1Zn higher than those of Pt/C catalyst.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Sciences
·
2025
·
IF 6.3
Qing Zhang,Yuting He,Jing Zhang,Yadong Li,Yanfen Fang,Yunzhi Tan
Enhancing the catalytic hydrolysis efficiency of microcystins (MCs) at ambient temperature has been a persistent challenge in water treatment. We employed N 2 /low-temperature plasma technology to modify the surface of natural pyrites (NP), and the resulting nitrogen-modified pyrites (NP N ) with a nanorod structure and new Fe-N x sites are more efficient for the hydrolysis of microcystins-LR (MC-LR). Kinetic experiments revealed that NP N exhibited significantly higher hydrolysis activity ( k obs = 0.1471 h −1 ) than NP (0.0914 h −1 ). Liquid chromatography-mass spectrometry (LC/MS) for the intermediates produced by hydrolyzing MC-LR, in situ attenuated total reflectance Fourier transform infrared spectroscopy (in situ ATR-FTIR) and X-ray photoelectron spectroscopy (XPS) analysis unfolded that the Fe and N atoms of Fe-N x sites on the surface act of NP N as Lewis acid and Brönsted basic respectively, selectively breaking amide bond on MC-LR molecule. This study demonstrates the effectiveness of plasma technology in modifying mineral materials to enhance their catalytic activity, providing a new method for eliminating MCs in practical water treatment.
研究领域:
环境科学
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水处理工程
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催化化学
✓ 已验证
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Qi Sun,Zhaoyang Wang,Min Zhou,Jiantao Li,Ruihu Lu,Yuhan Wang,Xiaobin Liao,Yan Zhao
Fe-N-C catalysts have been recognized as the most satisfactory candidates alternatively to Pt-based catalysts for oxygen reduction reaction (ORR). However, fine-tailoring of their intrinsic ORR catalytic activity still remains a great challenge due to the inferior accessibility and intrinsic activity of FeN x moieties. Herein, one order of magnitude activity enhancement of pristine Fe-N-C through cooperating with nitrogen-doped carbon micro-flower is achieved. The axial coordination effect between Fe active center and nitrogen atoms in support can break the electronic distribution symmetry of FeN x moieties and induce the electron delocalization on Fe active center and the electron localization on N, respectively, which favor the adsorption behavior of *OH intermediate. As a result, the catalyst exhibits a remarkable half-wave potential of 0.9 V and a high kinetic current density of 74.04 mA cm −2 at 0.85 V. In addition, when utilized as a cathode catalyst of liquid Zn-air batteries (ZABs), it possesses excellent electrochemical performance, for example, a high open circuit voltage (OCV) and peak power density of 1.59 V and 170.09 mW cm −2 , respectively. This work provides a new understanding into the activity enhancement mechanism of Fe-N-C catalysts, and inspires electronic delocalization of active sites for adjusting catalytic activity.
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 Sustainable Chemistry & Engineering
·
2019
·
IF 6.97
Xianliang Qiao,Chaoyue Zhao,Zhiqiang Zhou,Qingxin Guan,Wei Li
N-doped carbon material is a promising alternative to mercury catalyst for acetylene hydrochlorination. Herein, we present an innovative strategy to synthesize pyridinic N-rich aromatic ladder structure material through controlling the self-assembly of polyacrylonitrile polymer chains. The prepared material gave ∼93% conversion of acetylene with >99% selectivity for vinyl chloride and exhibited a satisfying stability during 200 h lifetime test. Characterizations and density functional theory calculations demonstrated that the activity of the catalyst likely originates from three types of active pyridinic N sites in the ladder structure. Particularly, the pyridinic N sites with one H atom nearby are more active because the H atom can stabilize the transition state through H···Cl bond, thereby reducing the energy barrier. The energy barriers on these pyridinic N sites were calculated to be 29.8 and 47.4 kcal mol–1, much lower than 83.2 and 84.4 kcal mol–1 on those sites without H atom nearby. The facile and highly effective strategy for the synthesis of a specific N species with defined formation mechanism is expected to be helpful in the design of other green catalysts for acetylene hydrochlorination.
研究领域:
材料科学
·
催化化学
·
理论计算化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）