Catalysis Science & Technology
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2023
·Vol. 14
·期 1
·110-118
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IF 5
Zi-Ye Liu,Qian-Yu Wang,Ji-Ming Hu
Modified NiFe-layered double hydroxide (NiFe LDH) materials with a high oxygen evolution reaction (OER) performance make it possible to replace noble metal catalysts for widespread applications. Herein, we prepare a layered carbon dot (CD) composite catalyst (denoted as NiFe LDH@CDs) by a one-step coprecipitation method without heating or hydrothermal treatment. Due to the numerous functional groups of CDs, there were strong electron interactions between the two components. The CDs promoted rapid charge transfers and accelerated OER kinetics. Moreover, through binding with the CDs, the NiFe LDH@CDs formed a heterojunction structure, which could efficiently suppress photoelectron–hole recombination. Based on the beneficial factors, the Tafel slope of NiFe LDH@CDs-200 was 44.77 mV dec−1, which further decreased to 38.44 mV dec−1 under light even with a low content of CDs.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Jiangfu Zheng,Changzheng Fan,Xiaoming Li,Qi Yang,Dongbo Wang,Abing Duan,Shuaijun Pan,Yuying Gao
The direct oxidative transfer process (DOTP) is a novel degradation-mineralisation system for the treatment of organic trace contaminants in water pollution, which are present with extremely high energy and/or chemical additions as well as large residues due to partial mineralisation. In this study, an enol-conjugated LDH (ACLDH) catalyst capable of interacting with persulfate was used, and tetracycline hydrochloride (TC) was degraded under visible light irradiation, and experimental and theoretical results showed that the ACLDH catalyst efficiently regulated its electrons. Under optimal experimental conditions, the ACLDH material acted as a catalyst to activate and stabilise the DOTP process on the surface of the nanocatalyst, resulting in the complete removal of TC within 35 min with up to 25 % mineralisation. In addition, the study investigated the effects of starting pH, catalyst dosage, several common inorganic anions and humic acid on TC removal. DOTP based on the ACLDH/PMS/Vis system is a very promising nanotechnology for water purification with strong performance in real waste leachate (up to 12 % TOC mineralisation) and disinfection applications.
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CHINESE JOURNAL OF CATALYSIS
·
2023
·
IF 16.5
Cheng Liu,Mengning Chen,Yingzhang Shi,Zhiwen Wang,Wei Guo,Sen Lin,Jinhong Bi,Ling Wu
Two ultrathin ZnTi-LDH nanosheets with different thickness (1.4 and 4.0 nm) were prepared to study the interplay between the active site and catalytic performance in photocatalytic synthesis of N -benzylideneanilline via a tandem reaction. ZnTi-LDH nanosheet possesses dual isolated active sites including the coordinatively unsaturated Ti atoms (Lewis acid sites) and the H atoms of OH groups (Brönsted acid sites), achieving the activation of benzyl alcohol and nitrobenzene via C–O···Ti species and N–O···H–O species, respectively. Photogenerated holes and electrons facilitate the oxidation of benzyl alcohol to benzaldehyde and the reduction of nitrobenzene to aniline, respectively. The thinner sample possesses more active sites, facilitating not only the activation of reactants but also the separation of photogenerated carriers. Therefore, a thinner ZnTi-LDH nanosheet shows the high conversion (100%) and the high selectivity (96%). Finally, a synergetic photocatalytic mechanism connected to the molecular activation is illustrated at the molecule level.
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ACS Applied Energy Materials
·
2023
·
IF 6.4
Junzhi Liao,Mengyao Xue,Yuankang Bao,Zhengtao Wu,Hao Zhang,Ping Li,Xun Xu,Shuwang Duo
The practical application of NiFe-based materials as high-performance water splitting electrocatalysts is severity restricted by their inferior hydrogen evolution reaction (HER) activity and long-term stability under large current density. Herein, we report a three-dimensional core–shell Ni/NiFe-layered double hydroxide (LDH) Schottky heterojunction on iron foam (Ni/NiFe-LDH/IF) electrode, in which a Ni metal nano-layer was directly deposited on the NiFe-LDH support grown in situ on commercial IF. Such an assembly enhanced the interfacial strength of the Ni/NiFe-LDH/IF electrode, promoted electron transfer and increased the adsorption energy of OH– as proved by density functional theory calculations. Consequently, the ultralow overpotentials (η) of 56 and 277 mV for HER and 140 and 330 mV for the oxygen evolution reaction (OER) resulted in the current densities of 10 and 1000 mA cm–2, respectively. The fabricated Ni/NiFe-LDH/IF two-electrode electrolyzer exhibited excellent water splitting characteristics, which produced the current densities of 10 and 1000 mA cm–2 at cell voltage of only 1.49 and 1.87 V, versus a reversible hydrogen electrode, respectively, which exceeded that of a commercial Pt/C||RuO2 catalyst. Moreover, the Ni/NiFe-LDH/IF electrolyzer demonstrated extremely high stability at 1000 mA cm–2 without a significant decay for more than 1500 h in a 1 M KOH solution and for 250 h at 60 °C in a 6 M KOH solution. This study proposes a scalable and extendable strategy for designing highly efficient and ultrastable electrocatalysts for hydrogen production at an ampere-level current density.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Yunpeng Liu,Zhongxin Chen,Yunyi Yang,Ren Zou,Binglu Deng,Linxin Zhong,Kian Ping Loh,Xinwen Peng
The major bottleneck in self-powered water splitting devices by renewable energy lies in the kinetically sluggish oxygen evolution reaction (OER), which only produces low-value oxygen. Herein, we explore sucrose electrooxidation as an alternative anodic reaction for production of valuable chemicals at a reduced electricity consumption. By developing a reversible redox cycle of Ni 2+ /Ni 3+ and Co 2+ /Co 3+ in the CoNi layered double hydroxide (LDH), the required voltage of sucrose oxidation for 100 mA cm −2 is reduced by 240 mV compared to oxygen evolution. The sucrose electrooxidation by CoNi LDH is a two-step reaction including the electrooxidation of Ni 2+ /Co 2+ to Ni 3+ /Co 3+ and the spontaneous reaction between Ni 3+ /Co 3+ and sucrose. By feeding with natural sugarcane juice, a solar-driven electrolyser is assembled for the co-production of value-added formic acid and hydrogen. Our work demonstrates a sustainable route for integrating hydrogen production and biomass electrooxidation for energy applications.
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JOURNAL OF ORGANOMETALLIC CHEMISTRY
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2018
·
IF 1.946
Jin Li,Yajuan Wang,Shunwang Jiang,Hui Zhang
A series of novel magnetic recyclable Pd Au nanoclusters (NCs) catalysts x-PdAu r /Fe 3 O 4 @LDH (x: Pd loading in wt%, r: Au/Pd molar ratio, LDH : layered double hydroxide, here refers the typical MgAl-LDH) were synthesized by a facile polyol reduction followed sol immobilization of PdAu r –PVP on core@shell support Fe 3 O 4 @LDH. Systematic characterizations reveal that the obtained catalysts possess the honeycomb-like core@shell, and the ultrafine PdAu alloy nanoclusters with the size in 1.70–2.55 nm highly dispersed on the LDH nanoplates shell. The obtained catalysts 1.0-PdAu r /Fe 3 O 4 @LDH (r: 0.11, 0.16 and 0.48) show higher Heck activity of iodobenzene with styrene than monomentallic ones, especially 1.0-PdAu 0.16 /Fe 3 O 4 @LDH displays the highest Heck activity under the optimal condition. Moreover, the catalysts can be applied for the Heck reaction of a variety of aryl halides with alkenes , and can be conveniently separated by an external magnet and reused ten runs without significant loss of activity.
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CHEMICAL ENGINEERING JOURNAL
·
2018
·
IF 6.735
Hua Tian,Wentao Bao,Yang Jiang,Lin Wang,Lin Zhang,Ou Sha,Cunqi Wu,Faming Gao
The ingenious synthesis strategies have been highly desired to construct hybrid composites with intriguing properties for supercapacitors . Herein, Ni-Al LDH (layered double hydroxide)/NNDG (nitramine-N-doped graphene) hybrid composites with a layered structure were fabricated via a novel self-assembly process. Nitramine-N dopants anchored to graphene framework allow the self-immobilization of delaminated Ni-Al LDH nanolayers onto the surface of two-dimensional carbonaceous scaffolds and boost the abundance of Ni 3+ within hybrid composites along with the removal of interlayer anions within Ni-Al LDH-NO 3 . Remarkably, the combination of Ni-Al LDH with NNDG can not only enhance the utilization of electrochemically active matrixes in dependence on the increase of electrolyte accessible active sites, but also maximize the electrochemically active contact between inorganic macromolecules and carbonaceous matrixes in favor of the establishment of conductive architectures. Furthermore, Ni-Al LDH/NNDG hybrid composites achieve a specific capacity of 975 C g −1 at a specific current of 1.0 A g −1 with a capacity retention of 75% as the increase of specific currents to 10 A g −1 , superior to Ni-Al LDH-NO 3 and Ni-Al LDH/rGO hybrid composites. The hybrid supercapacitor comprised of Ni-Al LDH/NNDG hybrid composites as a positive electrode and activated carbon as a negative electrode attains a high energy density of 59 Wh kg −1 with a power density of 1991 W kg −1 at a specific current of 2.5 A g −1 and retains 95% of the initial capacitance after 10 000 cycles at a specific current of 10 A g −1 . The excellence electrochemical performance demonstrates clearly the potential application of self-assembled Ni-Al LDH/NNDG hybrid composites for hybrid supercapacitors.
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Journal of Energy Storage
·
2025
·
IF 9.8
Peiyun Shu,Zhe He,Gentian Yue,Yueyue Gao,Jinghao Huo,Chen Dong,Furui Tan
The application of zeolite imidazole salt metal organic frameworks (ZIFs) and layered double hydroxides (LDHs) as bimetallic materials for supercapacitor electrodes is extensive, however, their inherent limitations hinder broader usage in supercapacitors. In this work, we developed a ZnNi-ZIF/LDH composite with a honeycomb structure through a sequential process involving ion doping and hydrolysis, utilizing ZIF-8 as a template to achieve a nanoscale honeycomb architecture. Subsequent phosphorization treatment yielded ZnNi-ZIF/LDH@P composite, further improving its conductivity. This process significantly enhanced the capacitive performance and stability of the composite electrode. The ZnNi-ZIF/LDH@P composite electrode revealed an excellent specific capacitance of 2855 F·g −1 at a current density of 2 A·g −1 , maintaining an impressive 93.4 % capacitance retention after 6000 charge-discharge cycles at a current density of 15 A·g −1 . The assembled ZnNi-ZIF/LDH@P//AC asymmetric supercapacitor was capable of powering a HENU light panel for at least 2 min, and its specific capacitance remained 96.4 % of the initial value after 4000 cycles at a current density of 5 A·g −1 . Overall, the ZnNi-ZIF/LDH@P composite demonstrates outstanding capacitance performance, highlighting its great potential in the field of energy storage.
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ANALYTICAL LETTERS
·
2024
·
IF 1.6
Haohua Wang,Le Ji,Yixiang Zhang,Ruotong Wang,Zheng Cao,Dong Wang,Junfeng Cheng,Chunlin Liu
Currently, the use of metal-organic framework (MOF)-based peroxidase (POD) mimics has been attempted for the development of colorimetric biothiol detection sensors. Furthermore, Ni/Co layered double hydroxides (NiCo-LDH), as sourced from MOF, have attracted increasing interest as enzyme mimics for colorimetric detection due to their low cost, adjustable layered structure, and composition. Herein, the hollow cubes of NiCo-LDH were synthesized with zeolitic imidazolate framework-67 (ZIF-67) as a sacrificial template. NiCo-LDH nanosheets were used to construct the hollow cubes with additional active sites exposed by the hollow structure. A series of experiments were conducted to confirm the superior catalytic activities of NiCo-LDH nanozymes as peroxidase (POD)-like inhibitors to horseradish peroxidase. The enzymatic kinetic constant Km values for NiCo-LDH nanozyme were 0.70 mM (H2O2) and 0.16 mM (TMB). Glutathione (GSH) was determined with a detection limit of 0.263 μM and a detection range from 5 to 60 μM. Meanwhile, the platform exhibited exceptional selectivity and stability. The mechanism and application of NiCo-LDH nanozymes were explored to promote the development of nanozymes with multi-metal active sites.
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Journal of Physical Chemistry C
·
2016
·
IF 4.509
Weiyang Lv,Qingqing Mei,Miao Du,Jianliang Xiao,Weijuan Ye,Qiang Zheng
To explore the influence of filler topological shape on the rheological behavior of poly(vinyl alcohol) (PVA) aqueous solution, three kinds (nanosized layered crystals, microsized layered crystals, and nanoscrolls) of layered double hydroxides (LDHs) were synthesized. Except for nanosized layered crystals, both LDH microsized layered crystals and nanoscrolls filled system showed distinct “N” shape viscosity curves with increasing LDH loadings. Notably, the one-dimensional LDH nanoscrolls could increase or decrease the viscosity of PVA solution by only changing the loadings. With combined theoretical calculation with dynamic mechanical analyses, the adsorbed state of PVA chains on surface of the three LDH particles was proposed, in which PVA chains exhibited various adsorbed states due to different interactions between PVA chains and LDH particles with disparate topological shape. Taking the advantage of remarkable rheological modulation and adsorption capacity, LDH nanoscrolls were introduced into PVA aqueous solution to broaden effectively its electrospinnable concentration window from 8.5–11.3 wt % to 6.5–18.0 wt %. More importantly, the adsorption capacity of LDH nanoscrolls was well preserved in the as-electrospun composite nanofibers, implying a superior adsorbent for methyl orange from wastewater was obtained.
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Surfaces and Interfaces
·
2024
·
IF 5.7
Zhuangzhuang Xiong,Ziheng Qi,Wenhui Zhang,Mingbo Ji,Fuqiu Ma,Lixia Ying,Guixiang Wang
Anodized aluminum, due to its inherent porous channels and thin protective layer, exhibits poor corrosion resistance and friction performance in severe environments. In this study, an in-situ growth of a NiZnAl-LDH composite coating was developed on the surface of aluminum. Sodium molybdate and ricinoleic acid were used to modify the coating, enhancing both corrosion resistance and friction performance. Various tests, including SEM, infrared, XPS, XRD, and others, were conducted to analyze the structure, composition, and properties of the synthesized coating. The results confirmed the successful synthesis of NiZnAl-LDH with nitrate intercalation, which were subsequently converted to molybdate intercalation through sodium molybdate modification. Electrochemical tests revealed that the corrosion current decreased by a factor of two compared to a plain LDH coating. Friction experiments demonstrated that the co-modified coating exhibited a minimal friction coefficient of 0.23, outperforming the original LDH coating.
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Desalination and Water Treatment
·
2025
·
IF 1
Yuyao Zhang,Yajie Li,Salma Tabassum,Gelan Zenebewerk Getachew
In this study, CO 3 2− intercalated Ni-doped CoMn layered double hydroxides were synthesized by co-precipitation method and used as peroxonosulfate (PMS) activation to degrade phenol efficiently. The physical and chemical properties of the catalyst were characterized by a series of methods. The effects of catalyst dosage, PMS concentration and initial pH value on phenol removal rate were investigated. The degradation mechanism was investigated by electron paramagnetic resonance (EPR) and quenching experiments. Experimental results indicated that the phenol removal is significantly impacted by the sulfate radical (SO 4 •− ), superoxide anion (O 2 •− ) and singlet oxygen ( 1 O 2 ). Furthermore, the inclusion of Ni stimulates the REDOX cycle of Co and Mn, and the activation of PMS to form active free radicals is caused by the REDOX cycle of Co 2+ /Co 3+ , Mn 2+ /Mn 3+ /Mn 4+ , Ni 2+ /Ni 3+ .
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