INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2023
·
IF 7.2
Haili Tong,Yi Jiang,Lixin Xia
The CQDs + Ni(OH) 2 /BiVO 4 photoanode was fabricated by introducing CQDs with fluorescence and optical properties . The CQDs + Ni(OH) 2 /BiVO 4 photoanode exhibited a low water oxidation onset potential (∼0.2 V vs. RHE) and a photocurrent density of 3.05 mA cm −2 at a voltage of 1.23 V vs. RHE, which is about 2.5 times than that of the unmodified BiVO 4 electrode, and the charge injection efficiency is 65%. Surface dynamics test showed that CQDs + Ni(OH) 2 /BiVO 4 photoanode had higher charge transfer rate and lower charge recombination rate than BiVO 4 electrode. As a cheap and stable catalyst for water oxidation, Ni(OH) 2 combined with CQDs can effectively improve the migration of photogenerated electrons and holes, thereby improving the photoelectrochemical (PEC) water oxidation activity of the photoanode.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2023
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IF 6.2
Hang Wang,Qing Sun,Yuanyuan Lin,Jian Zhang,Jiawei Sheng
Development of highly efficient and recyclable catalysts based on peroxymonosate (PMS) activation for the degradation of dangerous antibiotic contaminants was still a challenging topic. In this study, a highly efficient and recyclable heterogeneous Co(OH) 2 /ZnFe 2 O 4 (Co-ZF) catalysts derived from metal-organic frameworks (MOFs) were prepared by a facile alkaline solution hydrothermal method , a high specific surface area (100.4 m 2 g −1 ) and soft magnetic properties (Ms=25.3 emu g −1 ) composite material was obtained, and used for degrading norfloxacin (NOF) via PMS activation. The effects of temperature, alkali concentration, pH, initial NOF concentration, PMS and catalyst dosage on NOF degradation were discussed in detail. The results illustrated that the degradation rate of norfloxacin by the 3Co-ZF160 catalyst synthesized under 3 M NaOH and 160 ℃ hydrothermal conditions was 97.2%, after four consecutive cycles of degradation, the degradation rate of NOF by 3Co-ZF160 remained over 91% within 60 min. In contrast, the degradation rate of the Co 3 O 4 /ZnFe 2 O 4 (CZF-600) catalyst calcined at 600 ℃ was only 74% available. Furthermore, The results of radical quenching suggested that OH•, SO 4 • − , SO 5 • − and 1 O 2 functioned in the presence of the Co(OH) 2 /ZnFe 2 O 4 -PMS system. Eventually, NOF degradation pathways were tentatively proposed on the basis presented via LC-MS. The above results highlight that the practical application of Co(OH) 2 /ZnFe 2 O 4 heterogeneous catalyst in aqueous solution was of great significance.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Na Ye,Pengcheng Zhao,Xiaoying Qi,Riguang Zhang,Binhang Yan,Wenchao Sheng,Zhao Jiang,Tao Fang
Engineering high-performance inexpensive TaN-modified Pd-based nanostructures for alkaline methanol oxidation reaction(MOR) has attracted extensive attention, yet the related enhancement mechanism of TaN for MOR remains lacked. The core-shell like Pd 3 Ni 1 -TaN/C catalyst decorated with Ni(OH) 2 /NiOOH that contains highly dispersed Ni sites and nitrogen defects has been fabricated for the first time. The unsaturated coordination environment and core-shell like morphology of Pd 3 Ni 1 -TaN/C bring fruitful active sites and a down-shifted d -band center, making it a highly-efficient electrocatalyst for alkaline MOR (17.3-fold that of commercial Pd/C). Besides the electronic effects and surface defect sites of Pd 3 Ni 1 -TaN/C, TaN also helps MOR proceed via HCOO ad pathway (non-CO) accompanied by enhanced OH adsorption induced by the addition of Ni. DFT(Density Functional Theory) calculations also further confirm the energy barrier of the formation of HCOO ad intermediate and desorption energy of CO on Pd 3 Ni 1 -TaN/C are reduced. The introduction of Ni species and nitrogen vacancies enhances the CO tolerance evidently.
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INORGANIC CHEMISTRY
·
2022
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IF 5.436
Hu Yang,Aichuang Zhang,Yunfei Bai,Mingyu Chu,Han Li,Yuan Liu,Peng Zhu,Xiaolei Chen,Chengwei Deng,Xiaolei Yuan
Even though extensive efforts have been devoted to mixing Pd nanocrystals with Ni(OH)2 for the enhanced synergy, it remains a great challenge to incorporate nanosized Ni(OH)2 species on the Pd electrode and reveal their synergy. Herein, we present spongelike Pd nanocrystals with the modification of amorphous Ni(OH)2 species. The catalyst configuration is first considered by compositing Pd with Ni(OH)2 species to optimize the Pd–Pd interatomic distance and then constructing a strongly coupled interface between Pd nanostructures and Ni(OH)2 species. For the ethanol oxidation reaction (EOR) and the formic acid oxidation reaction (FAOR), Pd-Ni(OH)2 composites exhibit an impressive mass activity of 4.98 and 2.65 A mgPd–1, respectively. Most impressively, there is no significant decrease in the EOR activity during five consecutive cycles (50 000 s). A series of CO-poisoning tests have proved that the enhanced EOR and FAOR performances involve synergy between Pd nanostructures and Ni(OH)2 species.
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PubMed
高影响因子
NANOTECHNOLOGY
·
2022
·Vol. 33
·期 38
·385501
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IF 3.953
Yanxin Liao,Qian Du,Shupei Sun,Nianfeng Shi,Guangfu Yin,Zhongbing Huang,Xiaoming Liao
Self-supported Cu2S/Cu(OH)2 composite nanorods for highly sensitive non-enzymatic glucose sensing were in situ grown on Cu foam by simple hydrothermal treatment of aligned Cu(OH)2 nanorods. The physicochemical and electrochemical properties of the as-fabricated Cu2S/Cu(OH)2 composite nanorods were characterized by scanning electron microscopy, transmission electron microscopy, x-ray diffraction, Raman spectroscope, x-ray photoelectron spectroscope, cyclic voltammetry, electrochemical impedance spectroscopy, amperometric i–t measurements. The mechanism of the composite nanorods produced on conductive substrates was also explored. The electrode exhibits a sensitivity of 9626.88 μA mM−1 cm−2 towards glucose with good anti-interference ability, indicating it a promising electrode material for the enhanced non-enzymatic glucose detection.
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PubMed
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Chu Dai,Xike Tian,Yulun Nie,Wei Fu,Jiatang Wang
Most researches focus on design and optimization of heterogeneous Fenton catalyst itself to drive H 2 O 2 decomposition into • OH radicals. In this study, we reported the significant impact of the interaction mode of H 2 O 2 and CuMnO 2 (namely H 2 O 2 occurrence form) on the Fenton-like performance. The interaction mode of H 2 O 2 largely exposed to Cu atom active site (CMH-L) led to a superior ofloxacin (OFX) degradation efficiency of 93% compared with H 2 O 2 middle exposed around the Cu atoms (CMH-M, 84%) and small part exposed around the Cu atoms (CMH-S, 50%). The effect of H 2 O 2 occurrence forms on catalytic activity were confirmed by analyzing their fraction and the relevant rate constant with the correlation was 98%. And the relevant interfacial reaction mechanism was detailed explored based on density functional theory calculation, a series of probe experiments and quantitative analysis of H 2 O 2 utilization efficiency and • OH generation. It revealed that Cu atom arrangement on CuMnO 2 can induce the different H 2 O 2 occurrence form, and compared with CMH-M especially CMH-S (1.486 and 1.591 Å), CMH-L has the shortest elongation of O-O bond (1.477 vs. 1.468 Å in free H 2 O 2 ) together with the smallest O-H 1 and O-H 2 (0.988, 1.022 Å), which were more likely to decomposition H 2 O 2 into • OH, while it was more likely to inefficient transformation H 2 O 2 into O 2 in CMH-S system. Thus, this work provided a new insight for improving the heterogeneous Fenton catalytic performance via altering the interaction mode of H 2 O 2 and catalyst, which should be the fundamental reason for efficient H 2 O 2 activation into O 2 or • OH.
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CHEMOSPHERE
·
2022
·
IF 8.943
Shiwei Lai,Haiqian Zhao,Zhibin Qu,Ziyu Tang,Xue Yang,Peng Jiang,Zhonghua Wang
The mismatch of pollutant concentration and ·OH concentration is the key reason for the inefficient degradation of formaldehyde in the electro-Fenton system. Therefore, formaldehyde and ·OH are adsorbed near the cathode, and the high concentration reaction region is constructed to increase the reaction probability, which is called control of the reaction region. Through nitrogen doping modification of the activated carbon cathode, the adsorption capacity of the modified cathode for formaldehyde and active species, and the selectivity of the two-electron oxygen reduction reaction were deeply analyzed. The results show that the suitable nitrogen doping form of the modified cathode significantly promotes the adsorption capacity of formaldehyde and H 2 O 2 , which is beneficial to realizing the promotion of formaldehyde degradation by nitrogen doped cathodes in the electro-Fenton system through control of the reaction region. Graphite nitrogen and pyrrolic nitrogen improve formaldehyde adsorption by enhancing the van der Waals force (8.897 mg g −1 ), and pyridinic nitrogen improve H 2 O 2 adsorption (1.841 mg g −1 ) by enhancing the effect of hydrogen bonding interaction. Nitrogen doping enhances Fe 2+ regeneration, which contributes to the generation of ·OH at the cathode, and promotes formaldehyde degradation. The control of the reaction region through modification of the electro-Fenton cathode achieved formaldehyde degradation of 35.1 mg L −1 (48.51% higher than that of the unmodified cathode), which provides a promising process for formaldehyde treatment.
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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Xinjuan Du,Jindou Hu,Jing Xie,Aize Hao,Zhenjiang Lu,Yali Cao
The convenient modification of transition metal and the simultaneous adjustment of energy band are effective measures to improve the photocatalytic activity of titanium dioxide but remains challenging in photocatalytic hydrogen evolution field. Herein, In(OH) 3 -TiO 2 heterostructures were constructed by solid-state synthetic strategy under room temperature for tuning the band structure and accelerating the photoexcited charge separation to enhance the photocatalytic activity for hydrogen evolution. By the quantified modification of In(OH) 3 , the obtained In(OH) 3 -TiO 2 delivers an appreciable photocatalytic activity and stability for hydrogen evolution, which is 15.7 folds superior to commercial P25. Due to the narrowed band gap, the increased charge carrier density, the restrained recombination rate of photoexcited electron-hole pairs and the accelerated photogenerated charge separation, the In(OH) 3 -TiO 2 heterostructures thereby achieve the boosted photocatalytic hydrogen evolution performance. This work provides a feasible strategy to enhance the photocatalytic hydrogen evolution of TiO 2 via tuning the band gap and accelerating the photoinduced charge separation.
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ACS Applied Energy Materials
·
2022
·
IF 6.959
Mingxiong Lin,Ruodan Cao,Yifei Luo,Tingshi Zhang,Zanyong Zhuang,Yan Yu
Rational design of heterojunctions as photocatalysts that can help alleviate the energy and environmental crisis relies on the efficient electron transfer to the catalytically active sites. In this work, a robust metal–organic framework (MOF)-based heterostructured catalyst for the CO2 reduction reaction (CRR) was reported, taking advantage of a synergy effect between ultrathin (1.5 nm thickness) Ni-rich Ni(OH)2 nanosheets (NSs) and the highly stable and conductive Fe-rich Prussian blue (PB). This Ni(OH)2/PB photocatalyst can attain an optimal CO evolution rate of 108.8 mmol h–1 g–1 and a high CO selectivity (88.2–95.0%) in the CRR. The stable PB helps atomically thin Ni(OH)2 NSs to be well-dispersed and exposed in the heterojunction. A built-in electric field found at the interface of the bulk-sized PB and the ultrathin Ni(OH)2 further directs the electron transfer. Intriguingly, the conductive PB can quickly capture the electrons from the Ru-based photosensitizer and then rapidly sends them to the CRR-active Ni(OH)2 in the Z-scheme Ni(OH)2/PB system, accounting for its high efficiency and high selectivity over CO2 reduction into CO. The findings underline the versatility and the mechanistic response of MOFs in constructing advanced catalysts.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Wenbo Li,Difei Xiao,Xueqin Gong,Xianbin Xu,Fahao Ma,Zeyan Wang,Peng Wang,Yuanyuan Liu,Ying Dai,Zhaoke Zheng,Yuchen Fan,Baibiao Huang
Electrocatalytic polyethylene terephthalate (PET) waste upgrading is crucial for developing a circular plastics economy and solving the energy crisis, but achieving efficient PET upgrading at an industrial-scale current density remains a formidable challenge. In our work, Ni-MOF@MnCo-OH catalyst was prepared by designing hierarchical heterostructure and incorporating the concept of multi-metal sites, wherein the Ni-MOF can be derived from PET plastic. Benefiting from the advantages of material design, the catalyst demonstrates excellent adsorption capabilities for both OH ad and ethylene glycol (EG), while also enhancing the electron transfer capability of Ni-MOF. We achieve a high Faradaic efficiency (∼80 %) during PET plastic upgrading at industrial-scale current density (300 mA·cm −2 at 1.43 V vs. RHE) with Ni-MOF@MnCo-OH. Moreover, through theoretical calculations and in situ Fourier transform infrared (FTIR) spectroscopy, we have further elucidated the mechanism of ethylene glycol oxidation reaction (EGOR). Notably, glycolic acid has been identified as a vital intermediate during the electrical oxidation of EG. This work provides a viable and eco-friendly approach to enhance the value of PET waste through sustainable means.
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NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 48
·期 1
·228-236
·
IF 3.3
Yan Wang,Haoran Li,Daqing Chen,Danhua Ge,Xiaojun Chen
Herein, a simple solvothermal method was used to prepare a CuSx/g-C3N4 (CSG) heterojunction as an efficient oxygen activator containing sulfur vacancies (SVs). The as-prepared catalyst can activate oxygen to effectively degrade tetracycline (TC). The degradation rate of TC (20 mg L−1) reached 98.9% in 90 min over CSG (0.02 g L−1) under an air atmosphere, which maintained good performance within a wide pH range of 6–10. It was almost unaffected by any light source and water quality, indicating a highly efficient oxygen activator and good stability. Moreover, the trapping experiments and EPR results revealed that the main reactive oxygen species (ROSs) were singlet oxygen (1O2) and hydroxyl radicals (˙OH). CSG (4 : 1) enabled the activation of oxygen-produced ROS for removing TC even in the dark, which was in accordance with the EPR results. In addition, the CSG catalyst exhibited a good removal performance in practical wastewater treatment. Our study demonstrated that the CSG catalyst had the potential to remove organic pollutants from wastewater.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Jiani Zhang,Risheng Bai,Zhaochi Feng,Jiyang Li
Aiming to promote the activity of TS-1 zeolite in catalytic oxidative desulfurization (ODS), a general amide-assisted strategy was proposed to synthesize hierarchical TS-1 zeolite with rich and homogeneously distributed Ti(OH 2 ) 2 (OH) 2 (OSi) 2 species. Strong interactions between acrylamide (AM) and Si/Ti as well as self-polymerization of AM in synthetic gels change the zeolite formation process, thus to effectively construct Ti(OH 2 ) 2 (OH) 2 (OSi) 2 , promote Ti evenly distribution and form micro-mesopore structure. The activity of Ti(OH 2 ) 2 (OH) 2 (OSi) 2 was evaluated by ODS of refractory sulfur-containing compounds. The advantages of Ti(OH 2 ) 2 (OH) 2 (OSi) 2 over TiO 4 in substrate adsorption and reactive intermediate formation for ODS were further proved by theoretical calculations. By adjusting AM amount to optimize the Ti(OH 2 ) 2 (OH) 2 (OSi) 2 content and distribution, the obtained catalyst achieves 134.8 h -1 of turnover frequency and 100 % DBT removal at ten minutes, and maintains > 92 % removal after seven cycles at 333 K. This facile active-site construction strategy is promising to be extended to other heteroatom-containing zeolite catalysts.
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