INORGANIC CHEMISTRY
·
2019
·
IF 4.85
Wei Wang,Mehran Amiri,Tao Huang,Lev N. Zakharov,Yining Zhang,May Nyman
Isolating Fe(III) clusters from water without stabilizing ligands is significantly challenged by the high acidity of Fe3+-bound water, leading to uncontrolled precipitation of iron oxyhydroxides. Here we demonstrate a freeze-drying solvent-exchange method that enabled the isolation of a metastable Fe(III) sulfate decameric cluster formulated [Fe10O2(SO4)12(OCH3)2]·14CH3OH (Fe10). Without stabilization by solvent-exchange, the aqueous species undergoes rapid conversion to the iron sulfate mineral schwertmannite. Monitoring the hydrolysis process from cluster intermediates to schertmannite by small-angle X-ray scattering, we observe the progression from Fe10 to 37 Å soluble nanoparticles prior to the precipitation process. This condensation behavior of Fe10 is further exploited to develop a simple laboratory synthesis of schwetmannite. In addition, we demonstrate the versatility of the freeze-drying solvent-exchange method by isolating Al(III), Zn(II), and Cd(II) substituted Fe(III) sulfate clusters. The freeze-drying solvent-exchange method provides a unique opportunity to isolate cluster intermediates and models to aid in our understanding of metal-ion hydrolysis processes in environmental, material science, and geological studies.
研究领域:
环境科学
·
材料科学
·
地质学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Omega
·
2020
·
IF 2.87
Tianzhao Hu,Jiafu Chen,Xiaoqing Lu,Jing Chen,Zhimin Chen,Jianwei Fu,Yong Chen
Graphene sheets have a vast number of potential applications due to their excellent properties. However, poor quality and harsh preparation conditions restrict their application. Here, few-layer graphene (FLG) sheet powder with high quality has been synthesized from waste expanded polystyrene (EPS) at low temperature by dense Fe cluster catalysis. The micron-sized FLG sheets comprising about three layers show high crystallinity and good electrical conductivity that are comparable to those of the shear-exfoliated graphene nanoplatelets. More than 70% carbon yield of FLG sheets from cheap EPS and their safe, controllable synthesis conditions make it easy to expand production. The catalytic formation mechanism of FLG sheets is studied.
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
Nano Energy
·
2023
·
IF 17.6
Chunhui Wang,Keyi Xian,Shuangshuang Zhao,Shuailing Ma,Haozhe Qin,Dong Wang,Akhil Tayal,Yanfei Wang,Ying-Wu Lin,Ming Feng,Xing Ou
Interfacial engineering , especially atomic substitution at the interface or inside the nanomaterials , is a promising strategy for fabricating high-performance electrode materials. Herein, an interfacial modification strategy was reported to develop cobaltous sulfide (CoS 2 ) nanomaterials with Fe clusters modified on their interface and Fe single atoms partially substituted Co atoms in CoS 2 (Fe-CFS), which were further wrapped by graphene networks, forming highly active Fe-CFS@graphene nanomaterials (Fe-CFS@C) with triple reaction interfaces . As the 1st interface, graphene can decrease their electrical resistance. At the 2nd interface, partial substitution of Co atoms in CoS 2 by Fe single atoms can reduce its band gap and boost the potassium ion (K + ) diffusion rate. At the 3rd interface, anchoring Fe clusters on the surface of CoS 2 results in the formation of Schottky junction and promotes the formation of built-in electric fields, which accelerates the K + insertion/extraction kinetics and depresses the dynamic polarization. Acting as anode for K + battery , Fe-CFS@C exhibits a high reversible capacity of 755.8 mA h g −1 at 0.05 A g −1 . Even at 10 A g −1 , it can maintain 178.3 mA h g −1 over 4000 cycles due to the greatly enhanced electrochemical reaction kinetics and effectively improved structural stability.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Haoran Zhang,Yuelong Liu,Sanshuang Gao,Haijian Wang,Rui Bai,Yan Zhao,Yingtang Zhou,Guangzhi Hu,Xue Zhao
Green energy-driven electrochemical-nitrate-reduction-reaction (eNitRR) provides an alternative pathway for sustainable ammonia synthesis, but there is still a lack of reliable catalyst. Herein, through the combination of coordination confinement and spatial confinement, single-atom Fe and Fe clusters were simultaneously embedded on nitrogen-doped-hollow-carbon-tubes (Fe/NHCTs) to cooperatively promote the highly selective conversion of nitrate to ammonia in complex water environments. The ammonia yield rate reached 45595.63 μg h −1 mg −1 with Faradaic efficiency close to 100 %. The Zn-nitrate battery with Fe/NHCTs as the core has a high open circuit voltage and power density, and can output electric energy for a long time while highly selective synthesis of ammonia. The pathway and hydrogenation mechanism of nitrate evolution to ammonia were revealed using the in-situ attenuated total reflection Fourier-transform infrared, online differential-electrochemical-mass-spectrometry and density functional theory calculations, the intermodulation of electrons between single-atom Fe and Fe clusters synergistically accelerates the conversion of nitrate to ammonia.
研究领域:
材料科学
·
电催化
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
Science China-Chemistry
·
2024
·Vol. 67
·期 4
·1242-1249
·
IF 10.4
Zhang Jingjing,Deng Yongyan,Gai Dongxu,Shi Yang,Feng Xingwen,Li Peilong,An Yongtao,Zou Xiaoqin
Isotopic separation is of paramount importance for producing high-purity heavy hydrogen, yet the process remains hugely challenging. Here, we report on an Fe/ZSM-5 zeolite that was able to efficiently separate deuterium from protium via chemical quantum sieving. Structural data showed that four types of Fe species were present in Fe/ZSM-5 and oligomeric Fe–O clusters in the zeolite pores were correlated directly with gas selectivity. Gas adsorption revealed that Fe–O species served as the main adsorption sites and interacted with D 2 more strongly than with H 2 . D 2 /H 2 separation was exemplified using thermal desorption spectroscopy. D 2 /H 2 selectivity increased with Fe loading in Fe/ZSM-5 and a selectivity of 32.1 was obtained with an optimal loading of 7 wt%. The shift of desorption temperature supports the chemical affinity-based quantum sieving of D 2 over H 2 . This study demonstrates an effective strategy for enhancing D 2 /H 2 separation and the high selectivity means that Fe/ZSM-5 has strong potential in hydrogen isotope separation.
研究领域:
材料科学
·
物理化学
·
分离科学
·
催化化学
·
纳米材料
✓ 已验证
DOI
高影响因子
ENVIRONMENTAL RESEARCH
·
2021
·
IF 6.498
Xiang Liang,Wenhui Feng,Dong Liang,Yan Xu,Xiaoqing Qiu
Hydroxyl/amino and Fe(III) co-grafted graphite carbon nitride (CN) is fabricated via alkaline hydrothermal treatment and followed by an impregnation adsorption process. In this unique fabrication, hydroxyl and amino groups enriched on the surface play a vital role in improving the adsorption capacity for volatile organic compounds (VOCs), while the grafted amorphous Fe(III) clusters could dominantly regulate the path of molecular oxygen activation via photo-Fenton reaction, and change the selectivity of intermediate reactive oxygen species (ROS) with the assistant of the rich surficial hydroxyl groups. Meanwhile, both the grafted functional groups and Fe(III) clusters can serve as photogenerated charge acceptors for collaboratively accelerating carriers' separation. Besides, the Fe(III)-mediated interfacial charge transfer effect (IFCT) also could extend visible light absorption and boost carriers’ generation. Benefiting from the virtues of the complementary and synergy of the grafted hydroxyl/amino and Fe(III), the dual-functionalized CN is qualified as an efficient photocatalyst for removal of VOCs, which exhibits 22 and 18 times isopropanol (IPA) adsorption capacity and CO 2 production than of pristine CN during photocatalytic IPA removal, respectively. Moreover, this work provides a new strategy of surficial group-cluster bifunctionalization for systematically improving sustainable solar-to-chemical energy conversion towards VOCs mineralization.
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Sensors
·
2024
·
IF 8.2
Fan Shi,Zejun Zhang,Behisht Ara,Zhitan Huang,Qifeng Gui,Ahmad Mansoor,Wei Sun
Fe single-atom and Fe cluster-coupled N, S co-doped carbon nanomaterials (FeSA–FeONC-NSC) were prepared through a two-step high-temperature pyrolysis process using Gelidium corneum enriched with C, Fe, O, N, and S as precursors. The analysis by aberration-corrected scanning transmission electron microscopy and X-ray absorption spectroscopy revealed the presence of single-atom Fe in Fe–N4 coordination structures, along with small clusters as Fe–O-coordinated Fe2O3. Single-atom Fe in the form of Fe2+/Fe3+ provides more electrocatalytic active sites, which synergistically accelerates the charge migration process in the assembly of FeSA–FeONC-NSC with Fe2O3 clusters. The flexible nonenzymatic sensor, based on FeSA–FeONC-NSC and fabricated using a polydimethylsiloxane substrate, exhibited excellent catalytic activity for both uric acid (UA) and tyrosine (Tyr). Low detection limits for UA (0.14 μmol L–1) and Tyr (0.03 μmol L–1) were observed by using chronoamperometry in artificial sweat. The in situ detection of sweat was performed in combination with an integrated circuit board affixed to human skin, and the results were generally consistent with those of the high-performance liquid chromatography method. Therefore, FeSA–FeONC-NSC serves as a good modifier for wearable electrochemical sweat sensor applications.
研究领域:
材料科学
·
生物医学工程
·
分析化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-14
·
IF 15.7
He Zhe,Li Kailang,Chen Tianxiang,Feng Yunchao,Villalobos-Portillo Eduardo,Marini Carlo,Lo Tsz Woon Benedict,Yang Fuyuan,Zhang Liang,Liu Lichen
Liquid organic hydrogen carriers (LOHCs) are considered promising carriers for large-scale H 2 storage and transportation, among which the toluene-methylcyclohexane cycle has attracted great attention from industry and academia because of the low cost and its compatibility with the current infrastructure facility for the transportation of chemicals. The large-scale deployment of the H 2 storage/transportation plants based on the toluene-methylcyclohexane cycle relies on the use of high-performance catalysts, especially for the H 2 release process through the dehydrogenation of methylcyclohexane. In this work, we have developed a highly efficient catalyst for MCH dehydrogenation reaction by incorporating subnanometer PtFe clusters with precisely controlled composition and location within a rigid zeolite matrix. The resultant zeolite-encapsulated PtFe clusters exhibit the up-to-date highest reaction rate for dehydrogenation of methylcyclohexane to toluene, very high chemoselectivity to toluene (enabling the production of H 2 with purity >99.9%), remarkably high stability (>2000 h) and regenerability over consecutive reaction-regeneration cycles.
研究领域:
能源化学
·
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2020
·Vol. 8
·期 41
·21661-21667
·
IF 11.301
Dongchuang Wu,Xinyue Wang,Linghao Shi,Kaiyue Jiang,Mengjia Wang,Chenbao Lu,Zhenying Chen,Pan Liu,Jichao Zhang,Diana Tranca,Yang Hou,Yu Chen,Xiaodong Zhuang
Metal clusters with exposed atomic interfaces and unique electronic structures have received considerable attention in heterogeneous catalysis. However, their potential application in the electrocatalytic CO2 reduction reaction (CO2RR) remains very challenging because metal clusters tend to drive the competitive hydrogen evolution reaction. In this study, we prepared Fe-cluster sites with positive valence anchored on ordered mesoporous carbon materials for use as an efficient and durable electrocatalyst in carbon dioxide electroreduction. The as-prepared catalyst exhibits high selectivity, with a CO faradaic efficiency of higher than 98% at a low overpotential of 0.37 V, and retains 98.5% of its initial selectivity after 50 h of electrolysis in 0.5 M KHCO3. In addition, the as-prepared catalyst exhibits enhanced selectivity of more than 95% from −0.5 to −0.8 V in 0.1 M KHCO3, has 98.6% CO faradaic efficiency at a low overpotential of 0.49 V, and retains 99% of its initial selectivity after 50 h of electrolysis, thus outperforming state-of-the-art Fe–N-based single-atom catalysts. Density functional theory calculations revealed that the atomic interfaces on the Fe clusters reduce the reaction barrier for the *COOH intermediate, thus contributing to the rapid transformation of CO2 molecules and resulting in excellent catalytic performance.
研究领域:
电催化
·
多相催化
·
材料科学
·
环境化学
·
能量转换
✓ 已验证
DOI
高影响因子
Nature Communications
·
2022
·Vol. 13
·期 1
·1-11
·
IF 17.694
Wan Xin,Liu Qingtao,Liu Jieyuan,Liu Shiyuan,Liu Xiaofang,Zheng Lirong,Shang Jiaxiang,Yu Ronghai,Shui Jianglan
Simultaneously increasing the activity and stability of the single-atom active sites of M–N–C catalysts is critical but remains a great challenge. Here, we report an Fe–N–C catalyst with nitrogen-coordinated iron clusters and closely surrounding Fe–N 4 active sites for oxygen reduction reaction in acidic fuel cells. A strong electronic interaction is built between iron clusters and satellite Fe–N 4 due to unblocked electron transfer pathways and very short interacting distances. The iron clusters optimize the adsorption strength of oxygen reduction intermediates on Fe–N 4 and also shorten the bond amplitude of Fe–N 4 with incoherent vibrations. As a result, both the activity and stability of Fe–N 4 sites are increased by about 60% in terms of turnover frequency and demetalation resistance. This work shows the great potential of strong electronic interactions between multiphase metal species for improvements of single-atom catalysts.
研究领域:
化学
·
材料科学
·
能源科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nature Chemistry
·
2024
·
IF 19.2
Zhang Yangyu,Peng Xuanbei,Tian Han-Rui,Yang Bo,Chen Zuo-Chang,Li Jiejie,Zhang Tianhua,Zhang Mingyuan,Liang Xiaocong,Yu Zhiyang,Zhou Yanliang,Zheng Lirong,Wang Xiuyun,Zheng Jian-Wei,Tang Yu,Au Chak-tong,Jiang Lilong,Xie Su-Yuan
Developing highly effective catalysts for ammonia (NH 3 ) synthesis is a challenging task. Even the current, prevalent iron-derived catalysts used for industrial NH 3 synthesis require harsh reaction conditions and involve massive energy consumption. Here we show that anchoring buckminsterfullerene (C 60 ) onto non-iron transition metals yields cluster-matrix co-catalysts that are highly efficient for NH 3 synthesis. Such co-catalysts feature separate catalytic active sites for hydrogen and nitrogen. The ‘electron buffer’ behaviour of C 60 balances the electron density at catalytic transition metal sites and enables the synergistic activation of nitrogen on transition metals in addition to the activation and migration of hydrogen on C 60 sites. As demonstrated in long-term, continuous runs, the C 60 -promoting transition metal co-catalysts exhibit higher NH 3 synthesis rates than catalysts without C 60 . With the involvement of C 60 , the rate-determining step in the cluster-matrix co-catalysis is found to be the hydrogenation of *NH 2 . C 60 incorporation exemplifies a practical approach for solving hydrogen poisoning on a wide variety of oxide-supported Ru catalysts.
研究领域:
化学
·
材料科学
·
催化
·
氨生产
✓ 已验证
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）