ANALYTICAL AND BIOANALYTICAL CHEMISTRY
·
2022
·Vol. 414
·期 29
·8447-8461
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IF 4.478
Li Hui,Ma Chunxia,Gao Meng,Li Yong,Xie Lei,Zhao Dantong,Zhang Runhao,Zhang Guanhua,Li Wenhan,Rong Rong,Kong Biao
The inhomogeneous distribution of co-crystallized analytes and the traditional organic matrices as well as the intensive background interference in the low molecular weight range hinder the application of matrix-assisted laser desorption/ionization time-of-flight mass spectrometry (MALDI-TOF-MS) in the analysis of small-molecular compounds. New two-dimensional material MXene (e.g., Ti 3 C 2 ) exerts better hydrophilicity, homogeneity and repeatability, and higher laser desorption efficiency, as well as less background interference than traditional organic matrices and other nanomaterial matrices such as titanium oxide, graphene, and gold nanostructures. This study was aimed to design Ti 3 C 2 matrix with abundant hydroxyls on its surface, enhance the stability of this hydroxyl-rich Ti 3 C 2 (Ti 3 C 2 (OH) x ), and evaluate the analytical performances of Ti 3 C 2 (OH) x -assisted laser desorption/ionization time-of-flight mass spectrometry (LDI-TOF-MS) for small-molecular natural compounds in complex samples. The developed Ti 3 C 2 (OH) x showed the distinct advantages such as minimum background interference, high peak intensity (~10 5 ), high salt (0.6 M) and protein (0.5 mg/mL) tolerance, good repeatability (relative standard deviation<20%), and good stability after eight months of storage. Ti 3 C 2 (OH) x -assisted LDI-TOF-MS analysis could be used to rapidly identify Artemisia annua (a world-famous traditional Chinese medicine) and quantify the contents of the main chemical ingredients (oxymatrine (OXY) and matrine) of Compound Kushen Injection (CKI). Interestingly, the content of OXY in CKI could be accurately quantified by Ti 3 C 2 (OH) x -assisted LDI-TOF-MS, and there was a good linear relationship ( R 2 −0.9929), a low limit of detection (400 pg), and a low limit of quantification (600 pg) of OXY. Taken together, the rapid and accurate analysis of small-molecular natural compounds in complicated samples could be achieved by the Ti 3 C 2 (OH) x -assisted LDI-TOF-MS analysis. Graphical abstract
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高影响因子
NANOTECHNOLOGY
·
2023
·Vol. 34
·期 13
·135601
·
IF 3.5
Yudan Chai,Xuedong Wei,Yufen Wang,Shuangyan Qiao
In this paper, a Cr(OH)3 NSs@ZIF67 (NSs = nanosheets) electrocatalyst is prepared on foam Ni via a simple and rapid electrochemical deposition method. Excellent electrocatalytic activity of Cr(OH)3 NSs@ZIF67 is demonstrated. It can use the overpotential of 281 mV and 390 mV respectively to drive 10 mA cm−2 and 50 mA cm−2. It is observed that the Cr(OH)3 NSs@ZIF67 electrode has the highest initial current density at 1.57 V compared with the other two monomer electrodes and shows excellent stability at the end of 60 000 s. It has the largest electrochemical activity specific surface and lowest charge-transfer resistance, and M–O bonds (M = Co, Cr) and shifting of binding energy peaks at the interface lead to more active sites and more efficient electron transfer for oxygen evolution reaction. This work highlights the construction of highly efficient composite electrocatalysts composted of low-dimensional non-precious transition metal compounds and metalorganic frameworks, promoting the development of low-cost non-noble metal composites in energy chemistry.
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DALTON TRANSACTIONS
·
2022
·Vol. 51
·期 22
·8832-8839
·
IF 4.569
Yihao Gao,Jie Bai,Tianning Zhou,Yaqiong Gong
In recent years, Co-based metal–organic frameworks (Co-MOFs) have received significant research interest because of their large specific surface area, high porosity, tunable structure and topological flexibility. However, their comparatively weak electrical conductivity and inferior stability drastically restrict the application of Co-MOFs in the synthesis of electrocatalysts. In this study, ZIF-67 was grown on nickel foam by a room temperature soaking method, and then Ir–Co(OH)2@ZIF-67/NF was assembled by a hydrothermal method. The prepared Ir–Co(OH)2@ZIF-67/NF nanosheets exhibit remarkable conductivity, larger electrochemical active surface area and wider electron transport channels. Only ultralow overpotentials of 198 mV, 263 mV, and 300 mV were needed for Ir–Co(OH)2@ZIF-67/NF to reach the current densities of 10 mA cm−2, 50 mA cm−2, 100 mA cm−2, meanwhile, no obvious degradation of the current density at 10 mA cm−2 was observed for about 16 h. This work may provide a promising strategy for developing high-performance MOF-derived materials as electrocatalysts for the OER under alkaline conditions.
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Journal of Water Process Engineering
·
2022
·
IF 7.34
Jian Zhang,Yue Zhao,Maoxin Yang,Hong Jiang,Bing Wang,Yanping Jia,Weihua He
The abuse of doxycycline hydrochloride (DOX) in animal husbandry and its incomplete treatment have led to serious environmental problems, especially the risk of bacterial resistance. As an efficient, simple, and non-polluting method of catalysis, electrocatalysis has many advantages, which has attracted extensive attention in the removal of antibiotic pollutants in wastewater. Hence, the Ni/MWCNTs-OH/Ti composite electrode was prepared by galvanostatic electrodeposition to electrocatalyze DOX, and then the electrode was observed and analyzed by SEM , XRD and XPS. The optimal conditions (MWCNTs-OH was 0.10 mg/L, the concentration of NiSO 4 was 75 mmol/L, the degradation current was 15 mA, NaCl was present at a concentration of 0.20 mol/L, and pH value of 4) for degradation of 30 mg/L DOX within 60 min were determined by controlling variables. The degradation process of DOX followed Langmuir-Hinshelwood quasi-first-order reaction kinetics. As a result of stable the electrode, DOX removal rate was consistently above 70 % after 10 continuous uses, which showed good stability and reusability. The composite electrode electrocatalyzed DOX under the synergistic effect of cathode and anode. To identify the main intermediates involved in the electrochemical degradation of DOX, LC-MS was used. The toxicity of the intermediate products and final products was compared and analyzed by microbial culture experiment. And then Ecosar 2.2 was used to predict the biotoxicity of main intermediates to fish, daphnid, and green algae . This work provides a new material for the environmental remediation of antibiotic pollution.
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Nature Communications
·
2022
·Vol. 13
·期 1
·1-9
·
IF 17.694
Zhang Jiaxi,Zhang Longhai,Liu Jiamin,Zhong Chengzhi,Tu Yuanhua,Li Peng,Du Li,Chen Shengli,Cui Zhiming
The sluggish kinetics of the hydrogen evolution reaction in base has resulted in large activity gap between acidic and alkaline electrolytes. Here, we present an intermetallic IrMo electrocatalyst supported on carbon nanotubes that exhibits a specific activity of 0.95 mA cm −2 at the overpotential of 15 mV, which is 14.4 and 9.5 times of those for Ir/C and Pt/C, respectively. More importantly, its activities in base are fairly close to that in acidic electrolyte and the activity gap between acidic and alkaline media is only one fourth of that for Ir/C. DFT calculations reveal that the stably-adsorbed OH spectator at Mo site of IrMo can stabilize the water dissociation product, resulting in a thermodynamically favorable water dissociation process. Beyond offering an advanced electrocatalyst, this work provides a guidance to rationally design the desirable HER electrocatalysts for alkaline water splitting by the stably-adsorbed OH spectator.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Zepeng Rao,Guanhong Lu,Lu Chen,Asad Mahmood,Gansheng Shi,Zixia Tang,Xiaofeng Xie,Jing Sun
To identify the distinctive role of reactive oxygen species (ROS) and trace the intermediates not only help to decompose the pollutants in high efficiency but also for avoiding more harmful intermediates formed. Here, we developed a new method to generate different ROSs by controlling the atmosphere to distinguish their role in the degradation of flowing gas-phase VOCs, including o -xylene, styrene, and acetaldehyde. This method is in good agreement with the traditional sacrificial agent capture experiment. The results show that • OH radicals play a dominant role in the degradation of o -xylene and styrene, while • O 2 − radicals primarily take part in the acetaldehyde degradation. Additionally, we distinguish the role of holes, • OH and • O 2 − played during the VOCs photo-oxidation through the radical trapping, in situ DRIFTS, and GC-MS analysis. Under the attack of • O 2 − radicals, aromatic VOCs were photo-oxidized to intermediates containing benzene rings and ketones (i.e., toluene and butanone), while carbon chain compounds (i.e., 3-methylfuran and ethanol) tend to form under the action of • OH and holes. This can be associated with the different reaction paths initiated by ROS. For acetaldehyde removal, •O 2 − species facilitate the formation of acids (i.e., acetic acid) while the •OH species and holes lead to the production of ketones (i.e., acetone). This work provides deep understanding on the role of various ROS in the photocatalytic oxidation of VOCs, which can guide the design of efficient photocatalysts, selective formation of intermediates to be easily decomposed or as raw materials for further application.
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NEW JOURNAL OF CHEMISTRY
·
2021
·Vol. 45
·期 36
·16705-16713
·
IF 3.591
Xue Meng,Li Yan,Maobin Wei,Tao Wang,Ting Xu,Yongsheng Yan,Shihan Cheng
The developed peroxydisulfate (PDS) activation for removing pollutants is a significant technology. Here, a Co(OH)2/Cu2O composite was synthesized and used to activate PDS for tetracycline (TC) degradation. Covering the surface of Cu2O with Co(OH)2 could improve the stability of the material, reactive active sites, and electron transfer efficiency of the catalyst. Thus, Co(OH)2/Cu2O composite exhibited excellent performance in terms of degrading the TC pollutant, and in the Co(OH)2/Cu2O/PDS system, the removal rate of TC could reach 98% within 30 min. Moreover, the effect of pH value, PDS dosage, and TC concentration on the degradation efficiency of TC was systematically studied. According to free radical quenching experiments, the possible mechanism of TC degradation over the Co(OH)2/Cu2O/PDS system was proposed. This work provided a research basis for the use of metal oxides for PDS activation in environmental treatment.
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CHEMOSPHERE
·
2021
·
IF 7.086
Fang Zhu,Siyi Zhou,Mengying Sun,Jianfeng Ma,Wei Zhang,Kunjie Li,Hao Cheng,Sridhar Komarneni
Mg doped Ni(OH) 2 was synthesized and investigated as an efficient material to activate persulfate (PS) for phenol degradation. The property of the Ni(OH) 2 material was enhanced by Mg doping as the removal efficiency of phenol was increased from 74.82 % in Ni(OH) 2 /PS system to 89.53 % in Mg-doped Ni(OH) 2 /PS system within 20 min. Such a high removal efficiency revealed that doping Mg into Ni(OH) 2 brings about more defects (oxygen vacancies), which facilitated the formation of more active species in the degradation process. The removal efficiencies of phenol increased with the increase of the initial pH from 3 to 11. The influences of Cl − , NO 3 − and HCO 3 − on the stability of the system were also studied and the results showed that removal rates of all systems in the presence of these different inorganic anions could reached about 90 % within 20 min. Based on the electron spin resonance (ESR) experiments, 1 O 2 , O 2 ·- , ·OH and SO 4 •− were identified as the active species in Mg-doped Ni(OH) 2 /PS system for phenol degradation and a degradation mechanism was proposed for this system. In addition, the as-prepared material retained its activation performance even after 3 repeated cycles.
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ChemSusChem
·
2021
·Vol. 14
·期 14
·2935-2942
·
IF 8.928
Jifang Zhang,Wanbing Gong,Huajie Yin,Dongdong Wang,Yunxia Zhang,Haimin Zhang,Guozhong Wang,Huijun Zhao
Graphical Keep it 100 : A facile immersion approach has been developed to grow ultrathin nickel hydroxide nanosheets, which show excellent performance as the anode for electrocatalytic oxidation of 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid with 100 % yield and essentially 100 % faradaic efficiency under a low potential within a short reaction time. Development of electrocatalysts that are capable of efficiently oxidizing biomass-derived 5-hydroxymethylfurfural (HMF) into 2,5-furandicarboxylic acid (FDCA) is critically important for production of degradable plastics via non-fossil routes. In this study, a facile and scalable immersion synthetic approach has been developed to grow ultrathin nickel hydroxide nanosheets in situ on commercial nickel foam (Ni(OH) 2 /NF) as an anode for the electrocatalytic oxidation of HMF to FDCA with complete HMF conversion, 100 % FDCA yield, and >99 % faradaic efficiency at 1.39 V (vs. RHE) within 90 min. Mechanistic studies reveal that the initial oxidation of HMF takes place at the carbonyl group and FDCA is generated through two further oxidation steps. Impressively, the synthesized Ni(OH) 2 /NF can also be used to electrocatalytically oxidize other alcohol/aldehyde-containing compounds to the targeted products in alkaline medium with 100 % yield and >94 % faradaic efficiency under a low oxidation potential of 1.39 V (vs. RHE) within short reaction times.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Bo Lv,Xuefan Feng,Xiaoping Xi,Xinyan Feng,Zhenyu Yuan,Yu Yang,Fuqin Zhang
Heterogeneously structured materials with supported precious metals , such as Pd, Pt, and Ru, as co-catalysts are important catalysts for efficient photocatalytic water splitting. However, the high costs and low reserves of precious metals have been an obstacle to their application in hydrogen production . In this work, the noble-metal-free Cd 0.3 Zn 0.7 S solid solution was designed and synthesized with an optimized molar ratio of Cd/Zn for the best visible light photocatalytic performance. In addition, a heterojunction hybrid material formed between the Cd 0.3 Zn 0.7 S and Ni(OH) 2 nanosheet was engineered to improve the utilization of light and to inhibit the recombination of holes and electrons. Ni(OH) 2 nanosheets assisted the transfer of the photoexcited electrons to participate in the reduction reactions which is critical for efficient and rapid catalytic hydrogen production. The photoelectrochemical property of the hybrid material was investigated with UV–vis absorption, photoluminance (PL) and electrochemical impedance spectroscopy measurements. The mechanism of the high-efficiency and low-cost photocatalytic hydrogen production was established by analyzing the hydrogen evolution kinetics. With the success of replacing precious metal with nickel-based surface heterostructure, this work is expected to provide a new type of photocatalyst for the application of photocatalytic hydrogen production.
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Journal of Energy Chemistry
·
2021
·
IF 9.676
Zhiguo Zhang,Hua Huo,Zhenjiang Yu,Lizhi Xiang,Bingxing Xie,Chunyu Du,Jiajun Wang,Geping Yin
Mn doping is deemed as a promising strategy to improve the electrochemical performance of the α-Ni(OH) 2 battery-type supercapacitor electrode. However, the internal structure evolution, the pathways and the dynamics of the proton/intercalated anion migration, as well as the functioning mechanism of Mn dopant to stabilize the layered structure during cycles remain unclear. Here, we unveil that irreversible oxidization of Mn 3+ at the initial CV cycles, which will remain as Mn 4+ in the NiO 2 slabs after the first oxidization to effectively suppress the phase transformation from α-Ni(OH) 2 /γ-NiOOH to β-Ni(OH) 2 /β-NiOOH and further maintain the structural integrity of electrode. With a synergistic combination of theoretical calculations and various structural probes including XRD and 2 H MAS solid state NMR, we decode the structure evolution and dynamics in the initial CV (cyclic voltammetry) cycles, including the absorption/desorption of hydrogen containing species, migration of intercalated anions/water molecules and the change of interlayer space. This present work elucidates a close relationship between doping chemistry and structural reliability, paving a novel way of reengineering supercapacitor electrode materials.
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JOURNAL OF CLUSTER SCIENCE
·
2020
·Vol. 32
·期 5
·1371-1379
·
IF 1.731
Zhang Yingzhen,Song Yingying,Li Yancai
A simple and environment-friendly autocatalytic reduction process was developed for synthesis of Au/Ni(OH) 2 nanocomposites. The nanocomposites were characterized by scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). It is found the nanocomposites are composed of ultrathin Ni(OH) 2 nanosheets and gold nanoparticles (AuNPs), and the AuNPs disperse evenly on the Ni(OH) 2 nanosheets. The electrochemical and electrocatalytic properties of the Au/Ni(OH) 2 modified glassy carbon electrode (Au/Ni(OH) 2 /GCE) were investigated by electrochemical experiments. Furthermore, through optimizing Au loading of the nanocomposites, the 5%-Au/Ni(OH) 2 /GCE displays the best electrocatalytic activity towards glucose oxidization in alkaline medium. Under optimal conditions, the 5%-Au/Ni(OH) 2 /GCE displays a wide linear range of 0.01 to 3.15 mM (R 2 = 0.998) to glucose. Besides, the sensor has a low detection limit of 0.10 μM (S/N = 3) and a high sensitivity of 342.1 μA·mM −1 ·cm −2 . It also displays satisfying stability, good reproducibility and selectivity.
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