Environmental Technology & Innovation
·
2023
·
IF 7.1
Kaifeng Wang,Na Peng,Dongqing Zhang,Haijun Zhou,Jinfeng Gu,Jiahui Huang,Chen Liu,Yang Chen,Yang Liu,Jianteng Sun
This study investigated the adsorption performance of methylene blue using Ca(OH) 2 -modified biochar derived from agricultural and forestry wastes. The results showed that the modified rice straw biochar with 20% Ca(OH) 2 addition paralyzed at 500 °C exhibited the best adsorption performance for methylene blue. The adsorption data were fitted with four kinetic models and four isothermal adsorption models. Among which, the pseudo-second-order kinetic model and Langmuir isothermal model were the best fit, with high correlation coefficient of more than 0.99. The adsorption capacity of Langmuir fitting was 333.3 mg g −1 , which was 12.5 times higher than that for pristine rice straw biochar. The high adsorption capacity was maintained in a wide range of initial pH value of 4–12. SEM-EDX, organic element, surface structure, FTIR and XRD analysis indicated that Ca(OH) 2 modification significantly increased the polarity (higher O/C value), Ca content and the number of oxygen-containing functional groups (C-O and CO 3 2 − ) for pristine rice straw biochar, thereby substantially enhancing and improving the chemical adsorption of methylene blue. The adsorption mechanism involved for methylene blue included functional groups complexation, electrostatic interaction, ion exchange (mainly Ca 2＋ ) and π – π stacking. This study demonstrated that the modified rice straw biochar, as green and environmentally friendly raw material with cost-effectiveness, exhibited a great potential for broad application prospective subject to remediating printing and dyeing-contaminated wastewater.
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Biosensors-Basel
·
2022
·Vol. 12
·期 12
·1141
·
IF 5.743
Chunyuan Tian,Minggang Wei,Xiaobin Wang,Qing Hua,Feiyan Tang,Lijun Zhao,Xuming Zhuang,Feng Luan
In the present study, the electrochemiluminescence (ECL) properties of Gd(OH)3nanocrystals with K2S2O8as the cathode coreactant were studied for the first time. Based on the prominent ECL behavior of this material and the excellent specificity of the aptamer technique, an ECL aptasensor for the detection of ochratoxin A (OTA) was formulated successfully. Over an OTA concentration range of 0.01 pg mL−1to 10 ng mL−1, the change in the ECL signal was highly linear with the OTA concentration, and the limit of detection (LOD) was 0.0027 pg mL−1. Finally, the ECL aptasensor was further used to detect OTA in real samples (grapes and corn) and satisfactory results were obtained, which indicated that the built method is expected to be applied in food detection.Keywords:Gd(OH)3nanocrystals;electrochemiluminescence;aptasensor;ochratoxin A;food detection
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Haonan Ma,Chi Zhang,Long Chen,Mengning Xi,Zhiqiang Wang,Zheng Ni,Kecheng Zhu,Hanzhong Jia
Sorption processes at the mineral–water interface are of great importance in dominating the fate and availability of metalloid contaminants in natural environment. Aiming at a thorough understanding of the complexation of antimony (Sb) on metal hydroxide, we conducted first-principles molecular dynamic (FPMD) simulations and batch adsorption experiments to elucidate the quantitative mechanism of Sb complexation on Mg(OH) 2 . Batch experiments showed the sorption of Sb(III) is nearly pH-independent, while increasing pH markedly weakened Sb(V) sorption; the measured sorption isotherm curves were well fitted by Langmuir model. Subsequently, molecular-level mechanism of Sb(V)/Sb(III) on brucite basal and edge surfaces were revealed by FPMD, including microscopic surface reactive sites, local complexing structures and coordination geometries, and complexing free energies. Results showed that Sb(III)/Sb(V) can form outer-sphere complexation on basal surface by hydrogen bonding. On edge surface, Sb(III)/Sb(V) formed stable inner-sphere mononuclear monodentate and binuclear bidentate complexes. The calculated free energies indicated that the binuclear bidentate complexing was more favorable than monodentate structure, and the complexation of Sb(III) was more stable than Sb(V). Accordingly, reaction pathway of the ligand exchange and thermodynamic stability of the different inner-sphere complexes were clarified. This study provides theoretical basis for evaluating the environmental risk of Sb and improving the engineering efficiency of Sb-contaminated water management.
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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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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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Small
·
2022
·Vol. 19
·期 2
·2205719
·
IF 15.153
Wenjun He,Rui Zhang,Da Cao,Ying Li,Jun Zhang,Qiuyan Hao,Hui Liu,Jianling Zhao,Huolin L. Xin
Exploiting active and stable non-precious metal electrocatalysts for alkaline hydrogen evolution reaction (HER) at large current density plays a key role in realizing large-scale industrial hydrogen generation. Herein, a self-supported microporous Ni(OH) x /Ni 3 S 2 heterostructure electrocatalyst on nickel foam (Ni(OH) x /Ni 3 S 2 /NF) that possesses super-hydrophilic property through an electrochemical process is rationally designed and fabricated. Benefiting from the super-hydrophilic property, microporous feature, and self-supported structure, the electrocatalyst exhibits an exceptional HER performance at large current density in 1.0 M KOH, only requiring low overpotential of 126, 193, and 238 mV to reach a current density of 100, 500, and 1000 mA cm −2 , respectively, and displaying a long-term durability up to 1000 h, which is among the state-of-the-art non-precious metal electrocatalysts. Combining hard X-rays absorption spectroscopy and first-principles calculation, it also reveals that the strong electronic coupling at the interface of the heterostructure facilitates the dissociation of H 2 O molecular, accelerating the HER kinetics in alkaline electrolyte. This work sheds a light on developing advanced non-precious metal electrocatalysts for industrial hydrogen production by means of constructing a super-hydrophilic microporous heterostructure.
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LANGMUIR
·
2022
·
IF 4.331
Yibo Ao,Jinqing Ao,Ling Zhao,Liwei Hu,Fengsheng Qu,Biao Guo,Xue Liu
Cu(OH)2 nanomaterials are widely investigated for non-enzymatic glucose sensors due to their low-cost and excellent performance. Cu(OH)2 nanomaterials usually grow on substrates to form sensor electrodes. Reported works mainly focus on structure adjusting of the Cu(OH)2 nanostructures, while the optimization of substrates is still lacking. In the present work, directional porous Cu (DPC) was applied as the substrate for the growth of Cu(OH)2 nanograss (NG), and hierarchical structures of Cu(OH)2@DPC were prepared by alkaline oxidation. The morphology and microstructure evolution of the prepared hierarchical structures was investigated, and the non-enzymatic glucose sensing performance was evaluated. Cu(OH)2@DPC exhibits enhanced comprehensive non-enzymatic glucose sensing performance compared to the reported ones, which may benefit from both the effective adsorption of the Cu(OH)2 NG with a relatively high surface area and the high solute exchange of the DPC by a channel effect. This work provides new insights into the further improvement of the non-enzymatic glucose sensing performance of Cu(OH)2 nanostructures by optimizing the substrate structure.
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ANALYTICAL AND BIOANALYTICAL CHEMISTRY
·
2022
·Vol. 414
·期 29
·8447-8461
·
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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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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Catalysts
·
2023
·Vol. 13
·期 4
·715
·
IF 3.9
Dongrui Hou,Jing Luo,Qinggong Sun,Mengyang Zhang,Jianfeng Wang
In this study, Co-modified alkalinized g-C3N4(named Co-CNK-OH) was prepared for the Fenton-like photocatalytic degradation of tetracycline (TC) via a simple yet effective calcination–impregnation method. In all samples of CNK-OH with different Co2+loadings, Co-CNK-OH catalyst with the optimal content (9%) exhibited the highest catalytic activity, with 87.1% tetracycline removal and 50% removal efficiency of the total organic carbon (TOC). Mechanism studies revealed that the 9%Co-CNK-OH catalyst had the lower electrical resistance after alkalization treatment and Co2+modification, leading to a significantly accelerated interfacial charge transfer to the electron acceptor as well as effectively separating electrons and holes. The intermediates generated during the TC degradation in the photo-Fenton process were detected by HPLC-MS, which proved that the holes, superoxide radicals, and singlet oxygen are the key reactive species in the Fenton-like photocatalysis. This study provides a new option for the treatment of TC in wastewater.Keywords:Fenton-like photocatalysis;Co-CNK-OH;tetracycline;reactive oxygen species
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ACS Nano
·
2026
·
IF 17.3
Wenxiang Hou,Yusheng Zhang,Xuefei Chen,Xun Wang,Dayu Li,Wendai Cheng,Xixi Gong,Qu Wang,Ruofan Huang,Guanyuan Su,Chunmei Zhang,Liang Yang
Abstract Transition-metal hydroxides and oxides are widely used in optoelectronic and electrochemical devices, yet precise control over their three-dimensional (3D) microarchitecture and morphology remains a major challenge for microscale device fabrication. Here, we report a laser-confined interfacial nucleation and hierarchical growth (LCING) strategy that enables direct laser printing of Ni(OH)2/NiO microarchitectures with high spatial resolution and programmable porous structures. The localized photothermal field drives interfacial nucleation and hierarchical growth, allowing conformal integration of hydroxide microstructures and flexible construction of complex 3D geometries. We further elucidate the coupled mechanisms of mass transport, heat transfer, and reaction kinetics governing the LCING process. By rationally tuning laser printing parameters, the morphology and porosity of the resulting microstructures can be precisely controlled. The printed Ni(OH)2/NiO microdevices enable high-resolution structural color patterning and enhanced sensing performance, with the 3D porous Ni(OH)2/NiO architectures showing improved gas-sensing responses compared with lower-dimensional and nonporous counterparts. This work presents a versatile and programmable approach for high-precision manufacturing of functional metal-oxide microdevices.
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