ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Kun Lang,Yuanyingxue Gao,Xudong Xiao,Qi Li,Mingyang Liu,Jianan Liu,Huiquan Gu,Wei Wu,Huiyuan Meng,Baojiang Jiang
Seawater electrolysis offers a sustainable pathway for green hydrogen production, but chloride-induced side reactions, particularly chlorine evolution (ClER), limit the stability and efficiency of catalysts. Based on an interface-engineering strategy, a bifunctional CoP–MXene electrocatalyst was designed and fabricated, in which electrons are transferred from the Ti sites of the MXene support to the adjacent Co active centers of CoP. This directional electron donation modulates the Co electronic structure, generating electron-rich Co sites that effectively suppress Cl– adsorption via electronic repulsion while preserving the OH– reaction pathways through favorable proton–electron coupling. X-ray absorption fine structure (XAFS) spectroscopy, in situ Raman spectroscopy, and density functional theory (DFT) calculations further validate this electron modulation mechanism. In 1 M KOH electrolyte, CoP–MXene achieves a hydrogen evolution reaction (HER) overpotential of only 93 mV at 10 mA cm–2 and an oxygen evolution reaction (OER) current density of 50 mA cm–2 at 346 mV. In alkaline seawater, CoP–MXene exhibits exceptional HER performance (10 mA cm–2 @ 101 mV). Moreover, in an anion exchange membrane (AEM) electrolyzer (at 2 A cm–2 current density), the catalyst maintains over 500 h of stability in seawater with only 8.5% current decay, significantly outperforming the control samples. This study provides a new design strategy for the development of chloride-resistant electrocatalysts, advancing the application of seawater electrolysis technologies.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Peng-Fei Qiu,Xiu-Niang Tan,Zai-Yin Huang,Yan Zhou
The low conductivity of many traditional metal–organic-framework (MOF)-based electrode limits their developments in the field of electrochemical energy storage and still of great challenge. The controllable preparation of various kinds of nanomaterials using thiol-functionalized MOF shows great prospects. In this work, a thiol-functionalized metal–organic framework sheet structure ( Co-MOF/NF ) on nickel foam was successfully prepared by in situ interfacial growth synthesis, which was transformed into its derivatives S-doped β-Co(OH) 2 nanoflowers Co-x/NF ( x = 1, 2 and 6) in different concentrations of KOH solutions through ion etching/exchange reaction. The pristine thiol-functionalized Co-MOF/NF and its derivatives Co-x/NF ( x = 1, 2 and 6) nanoflower-like arrays could be used as positive electrode materials for effective supercapacitors. Among them, the transformation of the nanoflower-like Co-1/NF electrode exhibits excellent electrochemical properties with high areal capacitance (1925 ± 23 mF/cm 2 at 1 mA/cm 2 ), good rate performance, excellent conductivity and decent cycling stability. The Co-1//AC ASC device provides a high energy density of 0.176 mWh/cm 2 (92.6 Wh/kg) at a power density of 0.745 mW/cm 2 (392.1 W/kg). And this Co-1//AC ASC device exhibits a good cycling stability and practical application in energy storage field. This study provides a new strategy for the pristine thiol-functionalized MOF and its conversion nanostructures for energy storage applications.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Aiqun Kong,Mao Peng,Menghui Liu,Ye Lv,Houjun Zhang,Yusheng Gao,Jing Liu,Yan Fu,Wei Li,Jinli Zhang
Herein, we developed a novel and simple strategy to construct Pt-decorated TiO 2 /β-Ni(OH) 2 nanosheet arrays that steadily deliver large current densities in alkaline electrolyte. It is of great interest to find that the versatile role of few-layered Ti 3 C 2 endows the unique growth mechanism of Pt/TiO 2 /β-Ni(OH) 2 . It is worth noting that the interconnected array electrode exhibits noticeable hydrogen evolution reaction (HER) performance, achieving ultralow overpotentials of 107, 145 and 184 mV at high current densities of 500, 1000 and 1500 mA cm −2 , respectively, which outperforms most reported HER electrocatalysts. It requires only 1.95 V to drive 1000 mA cm −2 towards full water electrolysis along with considerable stability. It is demonstrated for the first time that the synergistic effect of Pt and TiO 2 /Ni(OH) 2 the enhanced HER performance. This work reports a robust nanoarray support for Pt electrocatalyst to break through its intrinsic barrier in alkaline HER and under large current density.
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ADVANCED MATERIALS
·
2018
·Vol. 30
·期 9
·1705366
·
IF 21.95
Dan Wu,Yicheng Wei,Xiang Ren,Xuqiang Ji,Yiwei Liu,Xiaodong Guo,Zhiang Liu,Abdullah M. Asiri,Qin Wei,Xuping Sun
It is highly desired but still remains challenging to design and develop a Co-based nanoparticle-encapsulated conductive nanoarray at room temperature for high-performance water oxidation electrocatalysis. Here, it is reported that room-temperature anodization of a Co(TCNQ) 2 (TCNQ = tetracyanoquinodimethane) nanowire array on copper foam at alkaline pH leads to in situ electrochemcial oxidation of TCNQ − into water-insoluable TCNQ nanoarray embedding Co(OH) 2 nanoparticles. Such Co(OH) 2 -TCNQ/CF shows superior catalytic activity for water oxidation and demands only a low overpotential of 276 mV to drive a geometrical current density of 25 mA cm −2 in 1.0 m KOH. Notably, it also demonstrates strong long-term electrochemical durability with its activity being retrained for at least 25 h, a high turnover frequency of 0.97 s −1 at an overpotential of 450 mV and 100% Faradic efficiency. This study provides an exciting new method for the rational design and development of a conductive TCNQ-based nanoarray as an interesting 3D material for advanced electrochemical applications.
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INORGANIC CHEMISTRY
·
2024
·
IF 4.3
Mengzeng Wu,Jingui Xu,Dongzhou Zhang,Yi Zhou,Wei Chen,Shanrong Zhang,Qifa Zhong,Dawei Fan
Layered materials have attracted extensive attention due to their exceptional physical and chemical properties. Understanding the structural evolution of such materials under high pressure is crucial for the development of new functional materials. In this study, the structure evolution of the synthesized layered rare-earth hydroxyhalide YCl(OH)2 under high pressures up to approximately 9.4 GPa was explored by using a diamond anvil cell combined with synchrotron single-crystal X-ray diffraction. Simultaneously, high-pressure Raman spectroscopy experiment was conducted to 10.3 GPa. Our findings indicate that YCl(OH)2 maintains its symmetry within the experimental pressure range. The pressure–volume data of YCl(OH)2 were fitted to the third-order Birch–Murnaghan equation of state (EoS) to derive its EoS parameters including zero-pressure unit-cell volume (VT0), isothermal bulk modulus (KT0), and its pressure derivative (K’T0): VT0 = 142.47 (1) Å3, KT0 = 38.2 (18) GPa, and K’T0 = 9.8 (1). However, the unit-cell parameters a, b, and c exhibit a distinct compressional behavior, with the a-axis being the most compressible and the b-axis being the least. Particularly noteworthy is the observation that YCl(OH)2 displays a negative linear compressibility along the b-axis within the pressure range of 0.4–5.3 GPa. Further detailed structure refinement and Raman spectroscopy analyses indicate that the anomalous behavior of the b-axis could be attributed to the formation of the O–H···O hydrogen bonding chains along the b direction. Moreover, the coordination number of Y3+ increased from 8 to 9 as the pressure reached 5.3 GPa due to the reduction of the interlayer spacing upon compression, ultimately leading to the closure of the interlayer gap.
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NEW JOURNAL OF CHEMISTRY
·
2024
·
IF 2.7
Fang Wu,Yuhong Jiao,Jinlong Ge,Yujun Zhu,chao feng,Zhong Wu,Chang-Peng Lv
Exploring highly active, low-cost electrocatalysts for oxygen evolution reaction (OER) is of great significance but still a major challenge. Here, we synthesized Ni(OH)2@Ni(Fe)OOH with a sea urchin structure on nickel foam via a simple hydrothermal and subsequent soaking process. Experimental results indicate that incorporation of Fe into Ni(OH)2 is favorable for modulate the electronic structure, faster electron transfer and improved intrinsic activity, thereby leading to excellent OER activity. The optimized Ni(OH)2@Ni(Fe)OOH exhibits superior OER activity with overpotentials of 245 and 310 mV at 10 and 100 mA cm-2, respectively, and a small Tafel slope of 40.7 mV dec-1, and along with high stability over 100 h, which is more active than benchmark RuO2 and sever control samples without introduction of Fe. More importantly, the overall water splitting system by using Ni(OH)2@Ni(Fe)OOH-100 as anode and Pt/C as the cathode only requires a cell voltage of 1.54 V to afford 10 mA cm-2. This work not only demonstrate the key factor of Fe doping, but also offers a new path for the development of NiFe-based OER catalysts.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Xinyu Guo,Jiaxin Li,Fanze Meng,Dongdong Qin,Xueyan Wu,Yan Lv,Jixi Guo
Properly design and manufacture of bifunctional electrocatalysts with superb performance and endurance are crucial for overall water splitting. The interfacial engineering strategy is acknowledged as a promising approach to enhance catalytic performance of overall water splitting catalysts. Herein, the Ru nanoparticles modified Ni 3 Se 4 /Ni(OH) 2 heterostructured nanosheets catalyst was constructed using a simple two-step hydrothermal process. The experimental results demonstrate that the abundant heterointerfaces between Ru and Ni 3 Se 4 /Ni(OH) 2 can increase the number of active sites and effectively regulate the electronic structure, greatly accelerating the kinetics of the hydrogen evolution reaction (HER)/oxygen evolution reaction (OER). As a result, the Ru/Ni 3 Se 4 /Ni(OH) 2 /NF catalyst exhibits the low overpotential of 102.8 mV and 334.5 mV at 100 mA cm −2 for HER and OER in alkaline medium, respectively. Furthermore, a two-electrode system composed of the Ru/Ni 3 Se 4 /Ni(OH) 2 /NF requires a battery voltage of just 1.51 V at 10 mA cm −2 and remains stable for 200 h at 500 mA cm −2 . This work provides an effective strategy for constructing Ru-based heterostructured catalysts with excellent catalytic activity.
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FUEL
·
2024
·
IF 6.7
Xiao Chen,Rongrong Li,Zhengwen Hu,Ying Zhong,Deng Hu,Changhai Liang
The selective activation of targeted bonds within renewable biomass-derived furanic compounds for the production of high-value alkyl diols holds significant importance for biomass upgrading, necessitating well-defined catalysts and clearly defined catalytically active sites. Herein, 1,5-pentanediol is synthesized through the selective hydrogenolysis of furfural-derived tetrahydrofurfuryl alcohol utilizing Ni-Co/La(OH) x bimetallic catalysts. The La(OH) x with abundant defect sites polarizes Ni-Co alloy for heterocracking of H 2 , as well as leads to expose more interfacial NiCo-O V -La 3+ sites. By harnessing the synergistic interplay between the alloy sites and the interfacial sites, the optimized Ni 4 Co 1 /La(OH) x bimetallic catalyst markedly enhances the adsorption of –OH groups in tetrahydrofurfuryl alcohol and facilitates the selective assault of active H species on the C-O-C bonds within tetrahydrofuran rings. This approach markedly elevates the selective hydrogenolysis of tetrahydrofurfuryl alcohol to 1,5-pentanediol, attaining an exceptional selectivity of 88.6 % with a conversion of 98.1 % for tetrahydrofurfuryl alcohol. Furthermore, the Ni 4 Co 1 /La(OH) x bimetallic catalyst demonstrates exceptional performance in the one-pot hydrogenation-hydrogenolysis of furfural to 1,5-pentanediol, exhibiting a low activation energy of 17.77 kJ/mol and a high turnover frequency of 192.1 h −1 . Notably, the Ni 4 Co 1 /La(OH) x bimetallic catalyst showcases remarkable stability. This outcome provides invaluable insights for the advancement of a sustainable process to produce diol monomers from renewable resources with a low carbon footprint.
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RSC Advances
·
2018
·Vol. 8
·期 7
·3611-3618
·
IF 2.936
Chenyang Zhang,Zhen Du,Ruyi Zhou,Peng Xu,Xinghua Dong,Yanyan Fu,Qing Wang,Chunjian Su,Liang Yan,Zhanjun Gu
Sparked by the growing environmental crises, photocatalytic degradation of chlorophenols with inexhaustible solar energy is expected to be converted into actual applications. Here, we report the preparation of the nanocomposite of Cu2(OH)PO4 and reduced graphene oxide (Cu2(OH)PO4/rGO) through a one-step hydrothermal method and examined its infrared-light photocatalytic activity in the degradation of 2,4-dichlorophenol (2,4-DCP). As evidenced by the absorption spectra and the degradation of 2,4-DCP, Cu2(OH)PO4/rGO exhibited enhanced infrared light-driven photocatalytic activity compared to pure Cu2(OH)PO4 and was very stable even after repeated cycling. More importantly, the introduction of hydrogen peroxide (H2O2) could combine the photocatalytic and photo-Fenton effects into one reaction system and maximize the infrared light photocatalytic efficiency. Typically, the rate constant of Cu2(OH)PO4/rGO and H2O2 was more than 6.25 times higher than that of only Cu2(OH)PO4/rGO, and almost 10 times greater than the value for pure Cu2(OH)PO4. Further, a plausible mechanism for the enhanced photocatalytic properties of Cu2(OH)PO4/rGO has been discussed. These findings may help the development of novel hybrid photocatalysts with enhanced infrared light photocatalytic activity for applications in the treatment of chlorophenol-contaminated wastewater.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Zhuoran Hou,Jie Yu,Xinsheng Zhou,Zhibin Chen,Jiawei Xu,Boyu Zhao,Wenbao Gen,Huayu Zhang
A self-supporting composite electrode material with a unique three-dimensional structure was synthesized by in-situ growth of nanoscale NiMnLDH-Co(OH) 2 on a nickel foam substrate via hydrothermal electrodeposition. The 3D layer of NiMnLDH-Co(OH) 2 provided abundant reactive sites for electrochemical reactions, ensuring a solid and conductive skeleton for charge transfer and resulting in significant enhancement of electrochemical performance. The composite material showed a strong synergistic effect between the small nano-sheet Co(OH) 2 and NiMnLDH, which promoted reaction kinetics, while the nickel foam substrate acted as a structural conductivity agent, stabilizer, and good conductive medium. The composite electrode showed impressive electrochemical performance, achieving a specific capacitance of 1870F g −1 at 1 A g −1 and retaining 87% capacitance after 3000 charge–discharge cycles, even at a high current density of 10 A g −1 . Moreover, the resulting NiMnLDH-Co(OH) 2 //AC asymmetric supercapacitor (ASC) demonstrated remarkable specific energy of 58.2 Wh kg −1 at a specific power of 1200 W kg −1 , along with outstanding cycle stability (89% capacitance retention after 5000 cycles at 10 A g −1 ). More importantly, DFT calculations reveal that NiMnLDH-Co(OH) 2 facilitates charge transfer, accelerating surface redox reactions and increasing specific capacitance. This study presents a promising approach towards designing and developing advanced electrode materials for high-performance supercapacitors.
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DALTON TRANSACTIONS
·
2022
·Vol. 51
·期 15
·5801-5809
·
IF 4.569
Yuan Yuan,Yuangang Xu,Qiang Xie,Dongxue Li,Qiuhan Lin,Pengcheng Wang,Ming Lu
A series of cyclo-N5−-based lead-containing energetic coordination polymers [Pb(OH)]4(N5)4 (1), [Pb3(N5)3(H2O)9(NO3)]4(N5)8(H2O)5 (2), [Pb(OH)]4(N5)3(NO3)(H2O)3 (3), and [Pb(OH)]4(N5)3(ClO4)(H2O) (4) were synthesized by self-assembly and characterized by single-crystal X-ray diffraction, powder X-ray diffraction, infrared and Raman spectroscopy, high resolution mass spectrometry, elemental analysis, scanning electron microscopy, and differential scanning calorimetry. In addition, their thermal decomposition kinetics have been studied theoretically and experimentally. The results revealed that the synthesized CPs possess regular structures, very high densities (2.852–4.537 g cm−3), good oxygen balances (CO2) (−2.72–+2.61%), good thermal stabilities (80–110 °C), and acceptable sensitivities (9.5–20 J; 120–240 N). This work will provide new inspiration for the development of cyclo-N5−-based coordination polymers and energetic materials.
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2022
·Vol. 169
·期 10
·106518
·
IF 4.386
Qingxiao Zhang,Pei Han,Hui Zhang,Jixin Yao,Xinyu Wang,Dongmeng Chen,Xueqin Zuo,Qun Yang,Shaowei Jin,Guang Li
The oxygen evolution reaction (OER) is a critical process in the operation of electrochemical water splitting. Metal-organic frameworks (MOFs) are applied in the field of OER electrocatalysis because of their unique structure, but the high impedance and unstable framework during pyrolysis remain unresolved. Here, MIL-88A (iron-based MOF) was modified by hydrolysis and loading Co(OH)2 to improve the catalytic activity. The electrochemical results showed that the Co(OH)2/MIL-88A achieved the optimized performance with the current density of 10 mA cm−2 at 278 mV (vs RHE). Density functional calculations (DFT) combined with characterization tests suggest that electrons transfer from Co(OH)2 to MIL-88A at the interface of the heterostructure, leading to a larger hole electron pair density. D-band theory calculations demonstrated that the synergistic effect of MIL-88A and Co(OH)2 in heterostructure strengthens the adsorption between active sites and adsorbate. The above proofs are the source of the excellent OER performance of the Co(OH)2/MIL-88A. The finding has certain reference significance for the heterogeneous treatment of iron-based MOF catalysts.
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