Catalysis Science & Technology
·
2026
·
IF 4
Tao Liu,Donglong Fu,Cuncun Wu,Xianhua Zhang,Gamal Sewify,Mohamed Mokhtar Mostafa,Sai Chen,Chunlei Pei,Zhi-Jian Zhao,Jinlong Gong
Hydroxy groups derived from water dissociation play a crucial role in reforming chemistry. A direct experimental verification of interfacial hydroxy groups, however, together with the precise control of active -OH species for hydrogen production has not been obtained. This paper describes an interface engineering strategy to modulate active -OH species for hydrogen production from methanol steam reforming. Based on comprehensive in-situ spectroscopic characterizations, the normalized bridged Ce3+-OH species present linear correlation with the copper-ceria interface density, suggesting that bridged Ce3+-OH species are mainly adsorbed at the copper-ceria interface. The bridged Ce3+-OH species adsorbed at interfacial sites are demonstrated as the primary active configurations that react with methoxy groups to generate formate species, thereby enhancing hydrogen production in low-temperature methanol steam reforming, achieving an optimal TOFH2 of approximately 956 h-1 at 220℃. This work provides a profound insight into the intrinsic reaction at the metal-support interfacial sites for the reforming chemistry.
✓ 已验证
DOI
高影响因子
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.
✓ 已验证
产品关联
DOI
高影响因子
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
✓ 已验证
产品关联
DOI
PubMed
高影响因子
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.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
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
✓ 已验证
产品关联
DOI
PubMed
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.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
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.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
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.
✓ 已验证
产品关联
DOI
高影响因子
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.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
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.
✓ 已验证
产品关联
DOI
高影响因子
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.
✓ 已验证
产品关联
DOI
高影响因子
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.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）