JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Ying Zhang,Rui Zhu,Jiang Zhong,Zhipeng Quan,Yongjian Zhu,Jingling Yang,Ping Liang,Jin Yong Lee,Hongguang Liu
Transition-metal-atom anchored graphdiynes (TM@GDY, TM = Mn, Fe, Co, Ni and Cu) have already been synthesized and found applications in hydrogen evolution , nitrogen fixation and etc. By means of first-principle predictions and test experiments, we propose here that Fe@GDY and Co@GDY are efficient catalysts for the sustainable conversion of O 3 to O 2 . These two catalysts can spontaneously chemisorb O 3 with zero reaction barrier and have low O 3 conversion barriers (0.31 eV and 0.19 eV, respectively). The O 3 decomposition experiment in a continuous flow membrane reactor and electron paramagnetic resonance results verify that Fe@GDY and Co@GDY are efficient catalysts under humid conditions. Raman spectra prove the formation of the key Fe-O/Co-O and Fe O O and Co O O intermediates. The hydrophobic nature of graphdiyne and the strongest chemisorption of O 3 among tested ambient gases, make Fe@GDY and Co@GDY ideal catalysts under both dry and humid conditions. These findings would stimulate future explorations on metal anchored GDY-based catalysts for applications of toxic gas decomposition or fixation.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2019
·
IF 5.155
Jianmin Chen,Hongtao Zou,Qilu Yao,Minghong Luo,Xiugang Li,Zhang-Hui Lu
The development of highly active, stable, and inexpensive catalysts for efficient and complete dehydrogenation of hydrazine is highly attractive but still very challenging. Herein, Cr 2 O 3 -modified NiFe (NiFe-Cr 2 O 3 ) nanopartciles (NPs) have been designed as the heterogeneous catalyst. Both the catalytic activity and hydrogen selectivity of Ni 0.9 Fe 0.1 -Cr 2 O 3 NPs were improved remarkably as compared with those of their mono-metallic counterparts. The prepared Ni 0.9 Fe 0.1 -Cr 2 O 3 catalyst exhibited an outstanding catalytic activity to release 3.0 equiv. (H 2 + N 2 ) from hydrazine in only 8.5 min at 70 °C, providing a turnover frequency (TOF) value of 893.5 h −1 based on surface metal atoms. Systematic studies indicated that the small size and high surface area of Ni 0.9 Fe 0.1 -Cr 2 O 3 as well as the strong synergistic electronic effect between Cr 2 O 3 and NiFe NPs resulted in the excellent activity of Ni 0.9 Fe 0.1 -Cr 2 O 3 catalyst. Such a highly rapid, long term durability, and low cost catalyst may encourage greatly the practical application of hydrous hydrazine as a chemical hydrogen storage material.
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
高影响因子
ADVANCED MATERIALS
·
2025
·
IF 26.8
Siyi Li,Jiaoting E,Xiucheng Zhao,Rui Xie,Jiaming Wu,Lili Feng,He Ding,Fei He,Piaoping Yang
Reactive oxygen species (ROS) play crucial roles in cellular metabolic processes by acting as primary intracellular chemical substrates and secondary messengers for cellular signal modulation. However, the artificial engineering of nanozymes to generate ROS is restricted by their low catalytic efficiency, high toxicity, and off-target consumption. Herein, hetero-trimetallic atom catalysts (TACs) anchored on a stable symmetrical pyramid structure are designed in the presence of N and P surface ligands from cross-linked polyphosphazene interlayer-coated MIL-101(Fe). The 3D network TACs with a uniform dispersion of Cu, Co, and Fe hetero-single atoms effectively tailor the active sites to avoid metal sintering, thereby providing sufficient catalytic activity for ROS blooms. Nanovesicle membranes facilitate the stable accumulation of nanozymes with homologous targeting, recognition, and endocytosis, effectively addressing the potentially high toxicity and off-target defects. Therefore, the outcome of the in situ ROS-bloom acts as a redox signal for directly regulating oxidative stress in the tumor microenvironment. Meanwhile, ROS intervene in the glutathione peroxidase 4, long-chain acyl-CoA synthetase 4, and cysteinyl aspartate specific proteinase-3 pathways as second messengers, fostering the proclivity toward apoptosis and lipid peroxidation-regulated ferroptosis pathway concurrently, thereby highlighting the application prospects of TACs in the biomedical field.
研究领域:
生物医学
·
肿瘤学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Catalysts
·
2023
·Vol. 13
·期 6
·931
·
IF 3.9
Junling Wei,Li Xu,Lihua Hu,Tiejun Wang,Yufei Ma
Hydrogen evolution reaction (HER) is a topic of great interest due to its efficient hydrogen production properties, which can address the increasing demand for clean and sustainable energy sources. On the other hand, molybdenum carbide (MoC) has been widely studied due to its noble metal-like surface electronic properties. In the HER process, it is crucial to regulate the Mo−H bonding energy effectively and increase the electron transfer rate on the MoC catalyst surface in a rational manner. In this study, we introduce highly electronegative nitrogen and non-noble transition metal atoms (Cu or Co) into the molybdenum carbide crystal lattice (N−M−MoC, M: Cu, or Co), which leads to a dual—doping effect. This effect results in the rearrangement of the electronic configuration on the catalyst surface and the enrichment of electrons around Mo atom, leading to an optimization in the Mo−H bonding energy. Moreover, the unique two-dimensional nano-sheet structure of the N−M−MoC materials further promotes the electron transfer and exposure of active sites. Benefiting from the above, the HER performance of the N−M−MoC is significantly improved. Among them, N−Cu−MoC exhibits the lowest overpotential (η10= 158 mV) and highest stability (about 30 h) in alkaline solutions.Keywords:dual-doping;heteroatoms;molybdenum carbide;hydrogen evolution reaction;surface electronic structure
研究领域:
材料科学
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催化化学
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能源科学
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry C
·
2024
·Vol. 12
·期 37
·14858-14864
·
IF 5.7
Qiang Liu,Jingnan Wang,Kaiheng Zhao,Yongan Yang,Xi Wang
Due to their well-defined geometric and electronic structures and fully exposed active sites, single-atom catalysts (SACs) exhibit significantly enhanced catalytic activity in the field of catalysis. However, the controllable synthesis of SACs, particularly in a simple and scalable manner, presents formidable challenges. Here, we report the general synthesis of SACs containing Co, Ni, Cu, and Zn using a direct impregnation method. Atomically dispersed transition metal atoms over zeolite supports are confirmed by integrated differential phase contrast scanning transmission electron microscopy (iDPC-STEM) and extended X-ray absorption fine structure (EXAFS) spectroscopy. Detailed studies reveal that the dispersion process originates from the trapping of metal atoms by silane nests. Notably, the Co-SAC catalyst demonstrated superior catalytic performance in the industrially significant propane dehydrogenation reaction. This synthetic strategy is straightforward and amenable to large-scale production of thermally stable SACs for industrial applications.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Qianqian Fu,Kunlun Nie,Min Wang,Xianguo Ma,Jianwei Ren,Mengqi Cui,Hui Wang
Efficient and cost-effective oxygen evolution reaction (OER) catalysts are crucial for advancing energy conversion and storage technologies such as water electrolysis and metal-air batteries. However, the performance assessment of catalysts has been complicated by the diversity of material microstructures and electrochemical testing variables. In this study, the solvothermal and chemical vapor deposition methods were employed to synthesize several NiCo-based compounds with similar microstructures but incorporating different non-metal atoms (O, P, S, and Se). By ensuring a comparable density of electrochemically active sites, the influence of non-metal atoms on the electronic structure and catalytic activity were investigated. Characterization and molecular orbital theory confirmed that electronic coupling enabled the redistribution of atomic charge transfer in the NiCo 2 S 4 (NCS) sample with bridging O 2- and S 2- . Electrochemical tests of the optimal catalyst in 1 M KOH demonstrated a lower Tafel slope (111 mV dec −1 ) and higher conductivity. The catalyst required only a 353 mV overpotential to achieve 100 mA cm −2 , and the subsequent chronoamperometry displayed a 98 % retention rate over 48 h. Such insights into the selection of non-metal atom provides a pathway for designing and preparing efficient catalysts.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
ChemNanoMat
·
2020
·Vol. 6
·期 8
·1191-1199
·
IF 3.384
Huixiang Li,Changhui Liang,Pan Gao,Guangjin Hou,Kairui Liu,Wei Liu,Qike Jiang,Shi Bai,Z. Conrad Zhang
Graphical In stock : Stock solutions of reduced mononuclear M 1 (0) (M=Pt, Au) atoms are prepared from their chloride salt precursors in removable solvent glycol ether/ethanol/H 2 O. Glycol ether and HCl function as strippable shields prevent M 1 (0) atoms from aggregation. The releasable M 1 (0) atoms suit as building-blocks for designable bottom-up material fabrications. Specifically, M 1 (0) atoms are readily transported onto the TiO 2 surface and remain in the reduced mononuclear state. Premade and readily transportable mononuclear zero-valent metal atoms in stock solvents offer the potential capability for bottom-up designable metallic material fabrication. This work demonstrates a potentially universal and practical strategy to prepare weakly shielded mononuclear metal atoms in a volatile solvent, which also constitutes a strippable ligand to the metal atoms. Herein, M 1 (0) (M=Pt, Au) atoms are prepared by reducing H 2 PtCl 6 and HAuCl 4 with ethanol in ethylene glycol diethyl ether (EGDE) under mild temperatures. The diether oxygens of EGDE, H + , and Cl − coordinating to the M 1 (0) atoms, make the M 1 (0) atoms stable in the solvent under low pH. However, the M 1 (0) atoms can be released either by evaporation of HCl and EGDE or through neutralization of the HCl with a base. The premade M 1 (0) atoms can be used as primary building blocks to construct designable materials. To demonstrate a potential application, the M 1 (0) atoms are conveniently transported onto the surface of TiO 2 through impregnation followed by mild heating. The atomic dispersion and reduced state of the metal atoms are well preserved, as verified by HAADF-STEM images, XPS, and DRIFT spectroscopy.
研究领域:
化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Sundaram Chandrasekaran,Na Li,Yang Zhuang,Lijun Sui,Zhizhong Xiao,Dayong Fan,Vanchiappan Aravindan,Chris Bowen,Huidan Lu,Yongping Liu
The creation of heterostructures based on non-precious metals with platinum-like hydrogen evolution reaction (HER) performance remains a challenge for hydrogen fuel technologies. Motivated by the fascinating properties of heterostructures, we establish here an effective approach to fabricate the heterostructured M−N−Ni 9 S 8 /Nb 2 O 5 ( M = Co, Fe, or Cu) catalysts using spatially separated Ni 9 S 8 nanosheet/Nb 2 O 5 nanobelts that are coupled with nitrogen (N) and metal atoms. Due to its improved intrinsic activity, interface-rich structure, abundant active sites, and large surface area the Co−N−Ni 9 S 8 /Nb 2 O 5 heterostructure achieved a low acidic HER overpotential of −171 mV at −10 mA cm −2 , thereby performing better than existing heterostructures. Moreover, for the alkaline HER, the Cu−N−Ni 9 S 8 /Nb 2 O 5 heterostructure required a low overpotential of −109 mV at −10 mA cm −2 , which is close to the performance of Pt/C catalyst. Density functional theory (DFT) predictions indicate that the local charge distribution and electronic properties at the heterointerface of Ni 9 S 8 /Nb 2 O 5 can be significantly modulated by co-doping of metals with N atoms, resulting in optimal adsorption energy and reduced water dissociation barrier; thereby accelerating the acidic and alkaline HER activity. This work, therefore, provides a new design principle to create advanced heterostructured catalysts.
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
Catalysts
·
2023
·Vol. 13
·期 7
·1118
·
IF 3.9
Yanling Wu,Qinggao Hou,Fangzhou Li,Yuanhua Sang,Mengyang Hao,Xi Tang,Fangyuan Qiu,Haijun Zhang
Biomass-derived porous carbon has gained significant attention as a cost-effective and sustainable material in non-noble metal carbon-based electrocatalysts for the oxygen reduction reaction (ORR). However, during the preparation of transition metal catalysts based on biomass-derived porous carbon, the agglomeration of transition metal atoms often occurs, leading to a notable decline in catalytic activity. In this study, we present a straightforward synthetic approach for the preparation of nitrogen-enriched soybean-derived porous carbon (Co@SP-C-a) as an electrocatalyst for the ORR. To achieve this, we employed a two-step method. In the first step, a chemical activator (KCl) was utilized to enhance the porosity of the self-doped nitrogen biomass carbon material. In the second step, a constant pressure drop funnel technique was employed to uniformly disperse bimetal cobalt/zinc-based zeolitic imidazolium frameworks (ZIF-L and ZIF-67) containing different metal ions (Zn2+and Co2+) into the activated biomass carbon material. Subsequent high-temperature calcination of the ZIF-L and ZIF-67@SP-C-a composite precursor yielded the Co@SP-C-a catalyst. The obtained catalyst exhibited remarkable ORR activity in an alkaline solution (Eonset= 0.89 V, E1/2= 0.83 V, JL= −6.13 mA·cm−2) and exceptional long-term stability. This study presents an effective strategy to prevent the agglomeration of metal nanoparticles when integrating them with biomass-based carbon materials, thus leading to enhanced catalytic performance.Keywords:transition metal atoms;biomass-derived porous carbon;chemical activator;oxygen reduction reaction
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 Energy Chemistry
·
2023
·
IF 13.1
Qingchun Zhang,Di Liu,Yaping Zhang,Zhiliang Guo,Minpeng Chen,Yuyun Chen,Bo Jin,Yingze Song,Hui Pan
The development of highly active, selective, and stable electrocatalysts can facilitate the effective implementation of electrocatalytic CO 2 conversion into fuels or chemicals for mitigating the energy crisis and climate problems. Therefore, it is necessary to achieve the goal through reasonable material design based on the actuality of the operational active site at the molecular scale. Inspired by the stimulating synergistic effect of coupled heteronuclear metal atoms, a novel Ni-Co atomic pairs configuration (denoted as NiN 3 ©CoN 3 -NC) active site was theoretically screened out for improving electrochemical CO 2 reduction reaction (CO 2 RR). The structure of NiN 3 ©CoN 3 -NC was finely regulated by adjusting Zn content in the precursors Zn/Co/Ni-zeolite imidazolate frameworks (Zn/Co/Ni-ZIFs) and pyrolysis temperature. The structural features of NiN 3 ©CoN 3 -NC were systematically confirmed by aberration-corrected HAADF-STEM coupled with 3D atom-overlapping Gaussian-function fitting mapping, XAFS, and XRD. The results of theoretical calculations reveal that the synergistic effect of Ni-Co atomic pairs can effectively promote the *COOH intermediate formation and thus the overall CO 2 RR kinetic was improved, and also restrained the competitive hydrogen evolution reaction. Due to the attributes of Ni-Co atomic pairs configuration, the developed NiN 3 ©CoN 3 -NC with superior catalytic activity, selectivity, and durability, with a high turnover frequency of 2265 h −1 at −1.1 V (vs . RHE) and maximum Faradaic efficiency of 97.7% for CO production. This work demonstrates the great potential of DACs as highly efficient catalysts for CO 2 RR, provides a useful strategy to design heteronuclear DACs, exploits the synergistic effect of multiple metal sites to facilitate complex CO 2 RR catalytic reactions, and inspires more efforts to develop the potential of DACs in various fields.
研究领域:
材料科学
·
环境科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Jingwen Wang,Qing Zhang,Lin Yang,Chuangang Hu,Zhengyu Bai,Zhongwei Chen
Interfacial hydrogen bonds are pivotal in enhancing proton activity and accelerating the kinetics of proton-coupled electron transfer during electrocatalytic oxygen reduction reaction (ORR). Here we propose a novel Fe Cr bimetallic atomic sites catalyst supported on a honeycomb-like porous carbon layer, designed to optimize the microenvironment for efficient electrocatalytic ORR through the induction of interfacial hydrogen bonds. Characterizations, including X-ray absorption spectroscopy and in situ infrared spectroscopy, disclose the rearrangement of delocalized electrons due to the formation of Fe Cr sites, which facilitates the dissociation of interfacial water molecules and the subsequent formation of hydrogen bonds. This process significantly accelerates the proton-coupled electron transfer process and enhances the ORR reaction kinetics. As a result, the catalyst FeCr N C achieves a remarkable half-wave potential of 0.92 V and exhibits superior four-electron selectivity in 0.1 M KOH solution. Moreover, the zinc-air battery assembled by FeCr N C demonstrates a high power density of 207 mW cm −2 and negligible degradation over 240 h at a current density of 10 mA cm −2 .
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
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2024
·
IF 11.2
Yike Huang,Cuihua An,Yafei Liu,Yusang Guo,Huaxu Shao,Huatang Yuan,Huaiyu Shao,Caiyun Wang,Yijing Wang
Herein, we report the multi-metal atomic catalysts for solid-state dehydrogenation of MgH 2 . It aims to reveal the multi-element synergy in catalysts for solid-state hydrogen storage. The kinetic measurements and fitting reveal two mechanisms: one shows a maximum rate at the early stage, such as V and Cr; the other needs a temperature-sensitive preparation time for its maximum rate, such as Ni. The combination of two catalyst components demonstrates the best kinetics: V and Cr boost the initial dehydrogenation, and Ni benefits the further hydrogen transfer which alleviates the rate of decay. This work provides guidelines for the design of multi-element doped catalysts for MgH 2 dehydrogenation.
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
危险品化学品经营许可证（带存储）