JOURNAL OF ALLOYS AND COMPOUNDS
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2022
·
IF 6.371
Wei Wen,Xiaoqiang Du,Xiaoshuang Zhang
Replacing fossil fuels by electrocatalytic water splitting for producing hydrogen and oxygen is one of the most promising ways to solve the energy crisis and environmental pollution. In this work, a series of M doped N-Ni 3 S 2 (M = Cu, Fe, Co and Ce) material was firstly synthesized and in situ grown on nickel foam substrate by a typical two-step hydrothermal synthesis method. Two probe reactions, water oxidation and urea oxidation, were selected to investigate the catalytic performance of these materials. What is noteworthy is that the Fe doped N-Ni 3 S 2 material exhibits superior water oxidation properties with requiring only 270 mV of overpotentials to drive current densities of 100 mA cm −2 , which is one of the best activities reported so far. After a long time of durability measurement, the current density of the Fe doped N-Ni 3 S 2 material will be attenuated, suggesting that the surface of the material will be in situ oxidized to oxide or hydroxide, which is the true active species. For urea oxidation, the Co doped N-Ni 3 S 2 material shows superior catalytic performance with requiring only 1.36 V potentials to drive 100 mA cm −2 current densities. Density functional theory (DFT) calculation shows that different adsorption energy of water for N-Ni 3 S 2 , N-Cu-Ni 3 S 2 , N-Fe-Ni 3 S 2 and N-Co-Ni 3 S 2 leads to the different catalytic activity. Experimental results demonstrate that the improved catalytic performance is assigned to faster electron transfer rates, exposure of abundant active center and better conductivity due to N and cation doping. This work provides new lessons for doping engineering for water splitting reactions.
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Surfaces and Interfaces
·
2024
·
IF 5.7
Yong Shi,Xin Lan Ma,Jin Suo Gao,Feng Yun Yu,Chun Yan Li,Wei Xiong,Li Ping Huang
The catalytic activity, adsorption and synergistic effect over bimetallic MOF derivatives with different dopant metal were systemically compared. A series of Me-Cu/TiO 2 (Me=Fe, Co, Ni) derived from bimetallic Me/Cu-BTC MOFs were fabricated via a sacrificing template method and applied for CO-SCR. Among the bimetallic catalysts, Fe-Cu/TiO 2 presented the best low-temperature of nearly 100% NO conversion from 150 °C to 350 °C with good NO selectivity. For Me-Cu/TiO 2 (Me=Fe, Co, Ni), the productions of crucial Cu + intermediate were determined to be 51.17%, 50.45%,49.4% by XPS, which were consistent with their catalytic activity results. The superior redox behavior of Fe-Cu/TiO 2 can be attributed to its higher Oβ / (Oα +Oβ) ratio of 32.90% and the higher Me 2+ / Me 3+ ratio of 1.79. In situ infrared analysis revealed that the Fe doping not only improved the formation and stability of nitrate species, but also enhanced the quantity of Lewis acid sites by forming Cu + -CO. Furthermore, a possible low-temperature Langmuir-Hinshelwood (L-H) mechanism over Me-Cu /TiO 2 (Me=Fe, Co, Ni) was proposed.
研究领域:
材料科学
·
环境催化
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Ying Fang,Qianwen Liu,Yang Song,Feiyue Jia,Ying Yang,Haipu Li
Dissolved organic matter (DOM) extensively exists in high-arsenic groundwater with relatively high concentration, which could not only compete with arsenic for adsorption sites, but also depress As(III) oxidation in persulfate-based advanced processes (PS-AOPs) through scavenging free radicals (SO 4 • − and •OH). In order to effectively avoid the negative effect of DOM , an Fe/Co bimetallic metal–organic framework (Fe/Co MOF)-coupled peroxymonosulfate (Fe/Co MOF-PMS) system was rationally constructed for non-radical-dominated As(III) oxidation and chemisorption-driven As(V) adsorption. Results showed that the Fe/Co MOF-PMS system did realize anti-interference As(III) immobilization in DOM-rich high-arsenic groundwater, which was evidenced by no difference in As(III) immobilization efficiencies in the absence and presence of 20 mg/L humic acid (HA). During the oxidation process, 1 O 2 dominated As(III) oxidation while O 2 • − dominated HA oxidation, and the presence of HA significantly promoted the generation of 1 O 2 besides SO 4 • − and •OH. During the adsorption process, chemical adsorption mainly drove As(V) adsorption such as forming M-O-As (M = Fe, Co) bond, while physical adsorption forces played a major role in HA adsorption, such as π-π interaction, hydrogen bonding, and electrostatic attraction. The synergism of oxidation and adsorption processes made the anti-interference As(III) immobilization in DOM-rich high-arsenic groundwater in Fe/Co MOF-PMS system come true. This work is believed to shed light on the highly efficient purification of DOM-rich high-arsenic groundwater.
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Molecular Catalysis
·
2023
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IF 4.6
Zizheng Zhu,Hongyan Zhang,Wen Guo,Hao Zhou,Yilin Zhou,Wenjie Liang,Maoshuai He,Wenxian Wei,Tingting Yu,Hong Zhao,Tao Yang
The highly efficient catalysts for the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) are of great significance for electrochemical water splitting. Direct transforming nickel foam (NF) into nickel-based catalysts attracts extensive attention because of its excellent stability and high conductivity. However, the catalytic performances of this kind of catalyst are still far from expected. Herein, we report a series of Ni oxides co-modulated by Mo, V and M ( M =Mn, Fe, Co, Cu) as efficient catalysts for water splitting, which are directly prepared through a simple NF-transformation method. Especially, a MoVNi catalyst displays a low Tafel slope of 68 mV/dec and a small overpotential of 76 mV at 10 mA/cm 2 for HER in 1.0 M KOH solution. The OER performances of MoVNi can be greatly enhanced by M introduction. For example, Fe-MoVNi only requires 374 mV to achieve 100 mA/cm 2 and shows no declination in a-20 h stability test at 100 mA/cm 2 in 1.0 M KOH media. Such performances outperform the recently reported best-performing Ni oxides catalysts in an alkaline environment. The excellent catalytic performances suggest great promise in practical applications.
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NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 18
·8739-8751
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IF 3.925
Quansheng Wu,Songhua Zhou,Chengbing Fu,Jiesong Zhang,Bo Chen,Hongyan Pan,Qian Lin
For the mono-metal Pd based catalysts, the O–O bond in O2 and H2O2 is easily dissociated due to the higher energy sites of Pd, which decreases the selectivity and productivity of H2O2. To address this issue, non-noble metals M (M = Sn, Fe, Co, Ni) were doped into palladium precursors to create a series of yolk–shell structure bimetallic catalysts Pd–M@HCS (H = hollow; C = carbon; S = sphere) with Pd–M as the core and porous carbon as the shell. The results indicated that the catalyst Pd–M@HCS doped with Sn, Fe, Co, and Ni has a weak dissociation ability for O2, and both the adsorption and dissociation ability for H2 are improved. Of these catalysts, the catalyst Pd–Sn@HCS gives the best performance, which is benefited by the suitable Pd–Sn nanoparticle size and the best Pd2+/Pd0 ratio. The influence of the nPd/nSn ratio in the Pd–Sn@HCS system on catalyst performance was further explored, and the findings revealed that Pd–Sn@HCS had the best catalytic activity and stability when the nPd/nSn ratio was 2. The catalyst's H2 conversion, H2O2 selectivity, and productivity were 35%, 97%, and 3961 mmol gPd−1 h−1, respectively. After 10 cycles, the H2O2 productivity of this catalyst remained at 92.1%, which was greater than the H2O2 productivity of the typical Pd-based catalyst Pd/C, which stayed at 37% under the same conditions.
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