Catalysis Science & Technology
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2024
·Vol. 14
·期 6
·1568-1578
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IF 4.4
Qifeng Chen,Peng Zheng,Haodi Liu,Yuanrong Zhang,Shuaitao Li,Hongpian Guo,Yanfen Fang,Xun Hu,Ran Duan
The combination of photocatalytic dehalogenation of halogenated aromatics and C–C coupling synthesis of valuable organics is an interesting method for the elimination of pollutants and synthesis of valuable chemicals. Herein, we present a green method for the photocatalytic dehalogenation of benzyl bromide and selective coupling synthesis of bibenzyl achieved on the dual active sites of single-atom Cu and surface oxygen vacancies (VOS) generated in situ on ultrathin 2D-TiO2(B) nanosheets. The experimental results show that single-atom Cu sites on ultrathin TiO2(B) nanosheets can improve charge transfer and separation efficiency and stabilize VOS formed in situ; the presence of VOS not only improves light absorption capacity but also favors the adsorption of reactant benzyl bromide molecules. More importantly, the dual sites of single-atom Cu and adjacent VOS form a solid frustrated Lewis pair, favor the adsorption of benzyl bromide molecules, activate the C–Br bond, and boost the C–C coupling synthesis of bibenzyl. This work provides a novel insight into photocatalytic C–C coupling through the synergistic effect of single-atom Cu and VOS on ultrathin nanosheet photocatalysts.
研究领域:
材料科学
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环境科学
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化学工程
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DOI
高影响因子
Korean Journal of Materials Research
·
2024
·Vol. 34
·期 9
·422-431
·
IF 0.3
Shu Ye,Jing Cheng,Zeda Meng,Won-Chun Oh
Hydrothermal and ultrasonic processes were used in this study to synthesize a single-atom Cu anchored on t-BaTiO3. The resulting material effectively employs vibration energy for the piezoelectric (PE) catalytic degradation of pollutants. The phase and microstructure of the sample were analyzed using X-ray diffraction (XRD) and scanning electron microscopy (SEM), and it was found that the sample had a tetragonal perovskite structure with uniform grain size. The nanomaterial achieved a considerable increase in tetracycline degradation rate (approximately 95 % within 7 h) when subjected to mechanical vibration. In contrast, pure BaTiO3 demonstrated a degradation rate of 56.7 %. A significant number of piezo-induced negative charge carriers, electrons, can leak out to the Cu-doped BaTiO3 interface due to Cu's exceptional conductivity. As a result, a single-atom Cu catalyst can facilitate the separation of these electrons, resulting in synergistic catalysis. By demonstrating a viable approach for improving ultrasonic and PE materials this research highlights the benefits of combining ultrasonic technology and the PE effect.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
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2025
·
IF 7.7
Yunpeng Xing,Sihao Zhi,Liang Zhao,Hongda Zhang,Chengchao Yu,Teng Fei,Sen Liu,Haiyan Zhang,Tong Zhang
The graphene-based room-temperature chemiresistive gas sensors have low sensitivity (especially for ppb-level organophosphorous compounds, OPCs), limiting their practical applications. Herein, a novel coupling single-atom Cu and N-enriched, π-conjugated carbon nanodots (NCDs) strategy is proposed to synthesize graphene-based sensing materials with excellent room-temperature DMMP sensing performances. Taking rGO-NCDs-Cu as the example, the N-enriched structures facilitate the adsorption of DMMP by providing more active sites and strengthening the hydrogen bonding interactions between -NH 2 and DMMP molecules. The π-conjugated structures can construct large π-delocalization network promoting charge generation and transport. The N-enriched and π-conjugated structures also result in narrowing band gap of NCDs, effectively enabling the increase of carrier transfer rate. Moreover, the introduction of single-atom Cu sites with Cu-N 2 Cl 2 structure further strengthens the hydrogen bonding interactions between sensing materials and DMMP molecules. Benefiting from this novel coupling strategy, rGO-NCDs-Cu sensor shows high response value of 13.95 % towards 340 ppb DMMP at room temperature. Meanwhile, rGO-NCDs-Cu sensor exhibits short response time (77 s) and recovery time (198 s), low practical limit of detection (34 ppb), excellent repeatability and high selectivity. Our work offers a new strategy for rational design of graphene-based materials for detection of OPCs at room temperature.
研究领域:
材料科学
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化学传感器
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环境监测
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Peizhen Yang,Yuhan Long,Wenli Huang,Dongfang Liu
Singlet oxygen ( 1 O 2 )-dominated advanced oxidation processes has drawn widespread attention for selective oxidation of organic pollutants in complex water environments. However, the high efficiency and selectivity of 1 O 2 generation remains challenging. Herein, we develop single-atom copper anchored on Ti 3 C 2 T x MXene nanosheets (Cu-SA/MXene) by molten salt etching for the generation of 1 O 2 via peroxymonosulfate (PMS) activation. Particularly, it exhibits a high selectivity of 99.71% toward 1 O 2 generation by activating PMS, which shows outstanding catalytic activity for multiple pollutants, and strong resistance to inorganic anions. Experimental and theoretical results reveal that the Cu single atoms with three oxygen coordination environments (Cu-O 3 ) are more favorable for PMS absorption and selectively adsorb the terminal oxygen of PMS to promote the generation of SO 5 .- , resulting in the generation of 1 O 2 . A continuous-flow wastewater system by dispersing catalysts on poly (vinylidene fluoride) membrane exhibit stable catalytic activity for polycarbonate plant wastewater treatment over 8 h.
研究领域:
环境科学
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材料科学
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催化化学
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产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2021
·
IF 10.588
Xue Zhao,Xue Li,Haibo Zhang,Xiao Chen,Jian Xu,Jun Yang,Hucai Zhang,Guangzhi Hu
Environmentally friendly electrochemical reduction pathways from NO 3 − to NH 3 or N 2 have provided feasible strategy into the green production of ammonia or the treatment of nitrate wastewater. Here, we anchored single-atom Cu with boron carbon nitride on carbon nanotube (BCN@Cu/CNT), and achieved the efficient operation of electrochemical nitrate reduction reaction (NIRR). BCN@Cu/CNT can efficiently catalyze the selective conversion of high-concentration nitrate into high-value-added ammonia, where the ammonia yield rate and Faradaic efficiency are as high as 172,226.5 μg h −1 mg cat. −1 and 95.32% (at −0.6 V), respectively. BCN@Cu/CNT also shows the ability to efficiently remove low-concentration nitrates in sewage. Specifically, here only takes 5 h to nearly 100% (99.32%) eliminate NO 3 - (50 mg L −1 ) in sewage without any residual NO 2 − . The excellent catalytic activity and physicochemical stability of BCN@Cu/CNT for NIRR suggest the promising industrial application prospects, including the green production of ammonia and the purification of nitrate wastewater.
研究领域:
环境科学
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电化学
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材料科学
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DOI
PubMed
高影响因子
ACS ES&T Engineering
·
2024
·
IF 7.4
Guangming Jiang,Zixun Liu,Shuxian He,Yinan Liu,Xiangyi Tang,Xiaoshu Lv,Fan Dong,Hong Liu
Electrocatalytic reduction of nitrate (NO3–) to ammonia (NH3) (NO3RR) coupled with NH3 separation represents a sustainable approach to mitigate nitrate pollution and recycle nitrogen from contaminated water. Nevertheless, this process is deemed impractical for contaminated natural water bodies owing to the limited presence of NO3––N (<50 mg L–1) and electrolytes and the relative abundance of scaling ions (Mg2+ and Ca2+). Furthermore, copper (Cu), as the primary NO3RR catalyst, generally suffers from NO2– accumulation and a prevalence of side hydrogen evolution. Herein, we develop an integrated system comprising sections of NO3– enrichment and NO3RR and NH3 collection, alongside a single-atom Cu-bearing CeO2 catalyst (Cu1/CeO2) for NO3RR. With this system, diluted NO3– is extracted from contaminated water using anion-exchange resins and then released into a concentrated NaCl aqueous solution, providing a solution with ample NO3––N (∼822 mg L–1) and electrolytes (∼1.7 M NaCl) while being free of scaling ions. Within this solution, the Cu1/CeO2 demonstrates an exceptional high and steady NH3–N production rate of 7.8 gNH3–N gCu–1 h–1, an NH3–N selectivity of 90.1%, and a Faradaic efficiency of 91.3%, outperforming the Cu nanoparticles (1.8 gNH3–N gCu–1 h–1, 46.3%, and 53.0%). In situ experiments and theoretical computations reveal a dual-site NO3RR mechanism involving the electron-deficient Cu1 site and adjacent oxygen vacancies, which collaborate to promote NO3– adsorption and lower conversion barrier while inhibiting hydrogen evolution. Finally, we implemented the integrated system along the Yangtze River, achieving nitrate elimination and nitrogen recycling with a competitive energy consumption of 1.36–1.54 kW h molN–1.
研究领域:
环境科学
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材料科学
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化学工程
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Di Zeng,Haipeng Wang,Xiaodi Zhu,Heng Cao,Yuanyi Zhou,Weimin Wang,Ling Zhang,Wenzhong Wang
Selective production of C 2+ chemicals from photocatalytic CO 2 reduction remains a big challenge due to the inert CO 2 molecular and vague C C coupling process. Herein, contributed by its uniform hexagonal pores, two-dimensional h'-H x WO 3 is selected as the support to realize single atom Cu loading (Cu/WO 3 ). Under the irradiation of light, the h'-H x WO 3 transformed into electron- and proton-rich tungsten bronze, which ensured the supply and transfer of multiple electrons/protons for the CO 2 reduction. Meanwhile, the similar coordination environment and appropriate distance of the Cu active sites presented by the Cu/WO 3 not only enable the adsorption and activation of CO 2 but also enhance the efficient C C coupling. Thus, Cu/WO 3 photocatalyst achieves the conversion of CO 2 to CH 3 COOH with a selectivity of 67 %, which is about 17 times higher than that of pristine h'-H x WO 3 . This work expands the route to prepare highly active single-atom catalysts, benefiting CO 2 photoreduction to selective reduction products.
研究领域:
材料科学
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环境科学
·
化学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Jinwen Hu,Xiangbin Cai,Jiao Wu,Cuncun Xin,Jingya Guo,Ziruo Liu,Jiazhen Wei,Xusheng Cheng,Ce Hao,Haopeng Dong,Guifeng Zhang,Ning Wang,Yongpeng Lei,Wei Liu,Yantao Shi
Endowing the transition-metal-nitrogen-carbon (M-N-Cs) electrocatalysts with high oxygen reduction activity for sustainable energy conversion, is a field of intense research while remains elusive. Here we exploit the variable configuration of atomically dispersed Cu 1 centers on carbon support via rationally constructing prototypical CuN 2+2 active sites to boost the kinetically sluggish electrochemical oxygen reduction. Density functional theory reveals the modified electronic structure of active Cu site and its derived orbital overlap through right symmetry with the degenerate π* orbital of O 2 molecule, which more effectively facilitates O 2 activation compared with CuN 4 counterpart. The targeted electrocatalyst delivers superior alkaline ORR activity with a half-wave potential of 0.88 V and superior kinetics with Tafel slope of 48 mV dec −1 , outperforming those of benchmark Pt/C. Remarkably, further demonstrated excellent peak power density and long-term durability in both primary liquid and flexible solid-state Zn-air battery assemblies signify the potential for practical applications.
研究领域:
材料科学
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电化学
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能源转换与存储
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DOI
高影响因子
ACS Catalysis
·
2024
·
IF 11.3
Heng Cao,Xiaodi Zhu,Jiawei Xue,Ruyang Wang,Jiusi Shang,Peiyu Ma,Chengyuan Liu,Jun Bao
Precise design of photocatalysts with the demanded active surface structure for highly efficient and selective CO2 photoreduction is crucial but challenging. Here, by taking CdS as a prototype, single-atom Cu is successfully constructed on Cd-deficient CdS (Cd1–xS) to improve the performance of CO2 photoreduction with H2O as proton donor. The optimal Cu/Cd1–xS with Cd vacancies (VCd)-mediated single-atom Cu exhibits nearly 100% selective CO production and a more than three-fold higher CO evolution rate compared to that of Cd1–xS. Both experimental identification and DFT theoretical simulation unveil that the VCd-mediated single-atom Cu render Cu–S pair sites to function as more catalytically active sites for dissociating H2O and promoting the corresponding proton supply, which favors the subsequent protonation of the adsorbed CO2 at the adjacent Cd sites via the two-proton coupled two-electron transfer pathway. This work demonstrates the importance of modulating proton supply from the oxidation half-reaction for facilitating the overall CO2 photoreduction, advocating an overall-reaction perspective for the design and development of highly efficient and selective CO2 conversion photocatalysts.
研究领域:
材料科学
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催化化学
·
理论计算
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产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Jiabai Cai,Huan Li,Qi Jing,Kai Feng,Masaki Takaoka
Landfill leachate is a refractory wastewater. Low-temperature catalytic air oxidation (LTCAO) has shown considerable potential for leachate treatment owing to its green and simple operation, but the simultaneous removal of chemical oxygen demand (COD) and ammonia from leachate remains challenging. Herein, TiZrO 4 @Cu SA hollow spheres with high-loading single-atom Cu were synthesized using isovolumic vacuum impregnation and co-calcination methods, and the catalyst was applied to the LTCAO treatment of real leachate. Consequently, the removal rate of UV 254 reached 66% at 90 °C within 5 h, while that for COD was 88%. Simultaneously, the NH 3 /NH 4 + (33.5 mg/L, 100 wt%) in the leachate was oxidized to N 2 (88.2 wt%), NO 2 - -N (11.0 wt%), and NO 3 - -N (0.3 wt%) owing to the effect of free radicals. The single-atom Cu co-catalyst in TiZrO 4 @Cu SA exhibited a localized surface plasmon resonance effect at the active center, which could quickly transfer electrons to O 2 in water to form O 2 .− with a high activation efficiency. The degradation products were determined and the deduced pathway was as follows: the bonds joining benzene rings were first broken, and then the ring structure was further opened to produce acetic acid and other simple organic macromolecules , which were finally mineralized to CO 2 and H 2 O.
研究领域:
环境科学
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催化化学
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产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Ge Fang,Ruonan Kang,Yu Chong,Liming Wang,Chuanqiang Wu,Cuicui Ge
In this study, the spatial location effect of the incorporated metal atoms on the hydrolysis activity of metal organic framework-based nanomaterials (MOFs) was investigated. UiO-type MOFs incorporated with single-atom Cu at different spatial positions were prepared and their hydrolysis activity towards phosphoester bonds was found to be highly depended on the location of the atomically dispersed Cu atoms. Especially, the attachment of Cu atoms to ligand (UiO-67-Cu N ) resulted in the most significant increase of their hydrolysis activity, which can be attributed to the elevated oxygen vacancies and increased Lewis acidity of MOFs. As a result, UiO-67-Cu N efficiently catalyzed the cleavage of DNA acting as DNA hydrolases, thereby effectively inhibiting the horizontal gene transfer of ARGs and eliminating bacterial resistance to antibiotic. This study opens up new prospects for the rational design of high-performance MOF-based DNA hydrolases and developing new treatment strategies for the removal of ARGs.
研究领域:
生物化学
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环境科学
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材料科学
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产品关联
DOI
高影响因子
ANALYTICAL AND BIOANALYTICAL CHEMISTRY
·
2024
·
IF 3.8
Wei Yuxin,Bai Qingqing,Ning Xinlu,Bai Xiaofan,Lv Jie,Li Meng
Sensitive and accurate detection of the amyloid-β (Aβ) monomer is of fundamental significance for early diagnosis of Alzheimer’s disease (AD). Herein, inspired by the specific Cu-Aβ monomer coordination, a cutting-edge colorimetric assay based on single-atom Cu anchored N-doped carbon nanospheres (Cu-NCNSs) was developed for Aβ monomer detection and an amyloidogenesis study. By directly pyrolyzing Cu 2+ -incorporated covalent organic frameworks (COFs), the resulting Cu-NCNSs with a high loading of Cu (8.04 wt %) exhibited outstanding peroxidase-like activity. The strong binding affinity of Aβ monomer to Cu-NCNSs effectively inhibited their catalytic activity, providing the basis for the colorimetric assay. The Cu-NCNSs-based sensor showed a detection limit of 1.182 nM for Aβ monomer, surpassing traditional techniques in terms of efficiency, accuracy and simplicity. Moreover, the system was successfully utilized for Aβ monomer detection in rat cerebrospinal fluid (CSF). Notably, the distinct inhibitory effects of monomeric and aggregated Aβ species on the catalytic activity of Cu-NCNSs were allowed for monitoring of the dynamic aggregation process of Aβ. Compared to thioflavin T (ThT), the most widely used amyloid dye, the detection system exhibited greater sensitivity towards toxic Aβ oligomers, which was crucial for early AD diagnosis and treatment. Our work not only sheds light on the rational design of highly active single-atom nanozymes from COFs but also expands the potential applications of nanozymes in early disease diagnosis. Graphical
研究领域:
生物化学
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医学诊断
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纳米材料科学
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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）