ACS Applied Energy Materials
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2024
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IF 5.4
Xiang Li,Zhitao Liu,Liyuan Zeng,Wanyi Ye,Guangxing Yang,Qiao Zhang,Shengjun Du,Zhiting Liu,Feng Peng
The CO2 electrochemical reduction (CO2ER) to produce valuable multicarbon products represents a promising approach for enhancing CO2 conversion. While previous research has investigated the impact of Cu electrode surface topography on C2 production, it is important to note that other parameters were also altered concurrently with changes in roughness. To isolate the specific effect of surface texture on CO2 electroreduction, this study prepared Cu layers with varying textures using the sputtering method with a varied sputtering time. To characterize the surface features of the sputtered Cu layers, the developed interfacial area ratio (Sdr), known as areal parameter, was introduced, with the aim of correlating it with C2 product selectivity. The results of this study indicate that the improved selectivity of C2 products can be attributed to higher Sdr values, primarily due to a rougher and finer surface texture that increases the local concentration of CO and OH–. This research underscores the significance of surface topography and offers perspectives for designing efficient Cu electrodes for the CO2ER.
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Journal of Environmental Sciences
·
2025
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IF 6.3
Yansen Qu,Xin Li,Yingjie Xia,Haosheng Lan,Le Ding,Jing Zhong,Xinghua Chang
Accelerated industrialization combined with over-applied nitrogen fertilizers results in serious nitrate pollution in surface and ground water, disrupting the balance of the global nitrogen cycle. Electrochemical nitrate reduction (eNO 3 RR) emerges as an attractive strategy to simultaneously enable nitrate removal and decentralized ammonia fabrication, restoring the globally perturbed nitrogen cycle. However, complex deoxygenation-hydrogenation processes and sluggish proton-electron transfer kinetics significantly hinder practical application of eNO 3 RR. In this study, we developed carbon-coated Cu-Ni bimetallic catalysts derived from metal-organic frameworks (MOFs) to facilitate eNO 3 RR. The unique structural features of catalyst promote enhanced synergy between Cu and Ni, effectively addressing critical challenges in nitrate reduction. Comprehensive structural and electrochemical analysis demonstrate that electrochemical nitrate-to-nitrite conversion mainly takes place on active Cu sites, the introduction of Ni could efficiently accelerate the generation of aquatic active hydrogen, promoting the hydrogenation of oxynitrides during eNO 3 RR. In addition, Ni introduction could push up the d-band center of the catalyst, thus enhancing the adsorption and activation of nitrate and the corresponding intermediates. Detailed reaction pathways for nitrate-to-ammonia conversion are illuminated by rotating disk electrode (RDE), in-situ Fourier-transform infrared spectroscopy, in-situ Raman spectrum and electrochemical impedance spectroscopy (EIS). Benefiting from the synergistic effect of Cu and Ni, optimum catalyst exhibited excellent nitrate reduction performance. This work provides a new idea for elucidating the underlying eNO 3 RR reaction mechanisms and contributes a promising strategy for designing efficient bimetallic electrocatalysts.
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ACS Nanoscience Au
·
2024
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IF 4.8
Dan Luo,Zhiheng Xie,Shuangqun Chen,Tianyi Yang,Yalin Guo,Ying Liu,Zhouhao Zhu,Liyong Gan,Lingmei Liu,Jianfeng Huang
Electrochemical semihydrogenation (ESH) of alkynes to alkenes is an appealing technique for producing pharmaceutical precursors and polymer monomers, while also preventing catalyst poisoning by alkyne impurities. Cu is recognized as a cost-effective and highly selective catalyst for ESH, whereas its activity is somewhat limited. Here, from a mechanistic standpoint, we hypothesize that electron-deficient Cu can enhance ESH activity by promoting the rate-determining step of alkene desorption. We test this hypothesis by utilizing Cu–Ag hybrids as electrocatalysts, developed through a welding process of Ag nanoparticles with Cu nanowires. Our findings reveal that these rationally engineered Cu–Ag hybrids exhibit a notable enhancement (2–4 times greater) in alkyne conversion rates compared to isolated Ag NPs or Cu NWs, while maintaining over 99% selectivity for alkene products. Through a combination of operando and computational studies, we verify that the electron-depleted Cu sites, resulting from electron transfer between Ag nanoparticles and Cu nanowires, effectively weaken the adsorption of alkenes, thereby substantially boosting ESH activity. This work not only provides mechanistic insights into ESH but also stimulates compelling strategies involving hybridizing distinct metals to optimize ESH activity.
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ENERGY & FUELS
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2024
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IF 5.2
Yongjin Wang,Zhipeng Zhou,Xiaoxia Zhang,Junjie Liao,Jiancheng Wang,Weiren Bao,Liping Chang
The preparation of a Cu-based sorbent supported by cost-effective AlOOH is proposed. A Cu-based sorbent for thiophene removal from coke oven gas was synthesized via coprecipitation, and the effect of AlOOH addition on the dispersion of activated Cu species and desulfurization properties was investigated. At an AlOOH content of 25%, smaller and more highly dispersed Cu grains, along with ZnO crystalline phases, were present on the surface of the Cu-based sorbent. The enhanced Cu-ZnO interaction contributed to the superior desulfurization performance (Qb-thiophene = 30.43 mg/g). The incorporation of an appropriate amount of AlOOH into the binary system during synthesis produces a highly active sorbent with superior Cu dispersion and smaller Cu grains, thereby fulfilling the requirements of industrial applications at a lower production cost.
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Inorganic Chemistry Frontiers
·
2024
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IF 6.1
Yifei Li,Senyao Meng,Ping Wang,Miao He,Jiasai Yao,Cheng Yang,Fangzhou Mo,Jiang Li,Zhenxing Li
The crystal facet of CeO2 is crucial in governing the catalytic performance of CeO2. However, studies on the relationship between the photocatalytic oxidation performance of CeO2 and its crystal facets are scarce. Herein, we synthesized a series of CeO2. Through loading Cu single atoms (Cu/CeO2), the facet effects of crystal facets on photocatalytic selective oxidation were systematically studied by employing the selective oxidation of 5-hydroxymethylfurfural to 2,5-diformylfuran as a model. Because the (110) facet's superior electron transfer efficiency is feasible for absorbing 5-hydroxymethylfurfural, eliminating α-H, and desorbing 2,5-diformylfuran, the selectivity of Cu/CeO2-nanorods (Cu/CeO2-R) with the (110) facet (93.34%) is much higher than that of Cu/CeO2-nanocubes (Cu/CeO2-C) with the (100) facet (32.22%) and Cu/CeO2-nanooctahedra (Cu/CeO2-O) with the (111) facet (15.20%). DFT calculation shows that Cu 3d exhibits orbital hybridization with Ce 5d and 4f, which provides a favorable pathway for electron transfer. This work delves into the facet-performance relationship during the photocatalytic process.
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LANGMUIR
·
2025
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IF 3.9
Lihuan Wang,Yanbing Dong,Liting Yuan,Xinxin Li,Yuan Li,Bingyan Li,Zijin Liu,Jinpeng Mo,Dongliang Dai,Xi Yu,Hui Yu
Inorganic nanofibers have emerged as a promising frontier in biomedical research thanks to their unique nanomorphology and bioactivity. Furthermore, the ions released from these inorganic biomaterials play a crucial role in determining cell identity and driving tissue-specific functions. Notably, Cu and Mn, which are essential trace elements in the human body, play significant roles in promoting bone health and participating in metabolic processes. Therefore, in this study, a series of Cu/Mn-doped SiO2–CaO composite nanofibers (CNFs) prepared by sol–gel electrospinning were obtained, and their morphology, flexibility, mineralization property, photothermal property, and antibacterial activity were studied. Experimental research has shown that the 2.5Cu and 2.5Mn CNFs calcined at 800 °C have the best flexibility, and as the Cu/Mn content or calcination temperature increases, the flexibility of CNFs decreases. In addition, 10Cu and 10Mn CNFs calcined at 800 °C have the best photothermal property, reaching temperatures of 65 and 62 °C under near-infrared irradiation (NIR) of 2 W cm–2 in the wet state, respectively, and the increase in calcination temperature results in decreased photothermal temperatures. The bacterial inhibition rates of CNFs (5Cu and 5Mn) with and without NIR are over 89 and 68%, respectively. The mineralization experiment also proved that Cu/Mn-doped CNFs have excellent mineralization activity. Therefore, these Cu/Mn-doped CNFs with excellent flexibility, photothermal property, mineralization activity, and antibacterial ability show great application potential in the treatment of tumors and bone defect-related diseases.
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ACS Applied Materials & Interfaces
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2024
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IF 8.3
Ze Li,Wen-Jie Li,Jun Guo,Zi-Yuan Wang,Xing Yang,Yu-Ke Zhu,Tian-En Shi,Yi-Xin Zhang,Jing Feng,Zhen-Hua Ge
SnSe materials have attracted extensive attention in thermoelectrics due to their low thermal conductivity. Nevertheless, the thermoelectric properties of n-type polycrystalline SnSe are still low, and metallic Sn distributed in the SnSe1–x materials would affect the repeatability of thermoelectric performance. Herein, the thermoelectric properties of n-type polycrystalline SnSe0.95-based composites are highly enhanced by heterogeneous Cu doping. The carrier concentration of the SnSe0.95 material was optimized by SnCl2 doping. The strategy of heterogeneous Cu doping is employed in further improving the thermoelectric performance of the SnCl2-doped SnSe0.95 materials. In addition, partial Cu+ doping tunes the electron concentration to enhance the Seebeck coefficient. Moreover, metallic Sn distributed along the grain boundaries can be stabilized by forming Cu6Sn5 alloys, which improve the thermal stability of bulk composites. Excessive Cu particles and SnCl2 precipitates strengthen phonon scattering for lowering the lattice thermal conductivity. Ultimately, a peak ZT of 1.55 is yielded at 773 K in the SnSe0.95–1 wt % SnCl2–1 wt % Cu bulk composite, whose mechanical hardness is also increased. Hence, these results promote a feasible approach to simultaneously enhance the thermoelectric and mechanical properties of n-type SnSe-based composites, which might be worth exploring in other thermoelectric materials.
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CHEMICAL PHYSICS LETTERS
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2024
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IF 2.8
Ye Liu,Lei Zhang,Yubo Kuang,Xiaoqian Xiang,Haohan Tao,Guangran Di,Xiaojing Yin,Meicheng Li,Xiao-Jun Lv
The photocatalytic CO 2 reduction has the problems of low selectivity of single product. Here, the preparation of Cu modified tubular C 3 N 4 (CTN) was studied. The increase of the active site inhibits the recombination of electrons (e-) and holes (h + ) and improves the selectivity of CO 2 reduction products. Finally, the CO and CH 4 yields of 1.5 % CTN photocatalyst are 11.55 μmol·g −1 and 4.72 μmol·g −1 , respectively, which are 5 times higher than that of tubular C 3 N 4 photocatalyst. The selectivity of 2 % CTN to CH 4 is up to 68 %, indicating that the prepared CTN photocatalyst has high CO 2 reduction activity and CH 4 selectivity.
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ENVIRONMENTAL RESEARCH
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2024
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IF 7.7
Lan-Ying Liu,Min-Hua Cui,John Justo Ambuchi,Shi-Ming Niu,Xin-Hui Li,Wo-Long Wang,He Liu,Guo-Shuai Liu,Ai-Jie Wang
Electrocatalytic hydrodechlorination (EHDC) is a promising approach to safely remove halogenated emerging contaminants (HECs) pollutants. However, sluggish production dynamics of adsorbed atomic H (H* ads ) limit the applicability of this green process. In this study, bimetallic Pd–Cu@MXene catalysts were synthesized to achieve highly efficient removal of HECs. The alloy electrode (Pd–Cu@MX/CC) exhibited better EHDC performance in comparison to Pd@MX/CC electrode, resulting in diclofenac degradation efficiency of 93.3 ± 0.1%. The characterization analysis revealed that the Pd 0 /Pd II ratio decreased by forming bimetallic Pd–Cu alloy. Density functional theory calculations further demonstrated the electronic configuration modulation of the Pd–Cu@MXene catalysts, optimizing binging energies for H* and thereby facilitating H* ads production and tuning the reduction capability of H* ads . Noteably, the amounts and reduction potential of H* ads for Pd–Cu@MXene catalysts were 1.5 times higher and 0.37 eV lower than those observed for the mono Pd electrode. Hence, the introduction of Cu into the Pd catalyst optimized the dynamics of H* ads production, thereby conferring significant advantages to EHDC reactions. This augmentation was underscored by the successful application of the alloy catalysts supported by MXene in EHDC experiments involving other HECs, which represented a new paradigm for EHDC for efficient recalcitrant pollutant removal by H* ads .
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CHEMICAL ENGINEERING JOURNAL
·
2025
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IF 13.2
Jiankang Wang,Shuhong Liu,Ping Song,Xiao Zhang,Ying Song,Wanqian Guo,Zhongping Yao
Nanoparticle aggregation and metal ion leaching contribute to the poor cycling stability of nanostructured zero valent copper (ZVC) catalyst for molecular oxygen activation, greatly hindering its industrial application in wastewater treatment. Herein, N doped carbon coated Cu 0 (Cu@CN) catalysts were prepared by using polyvinylpyrrolidone (PVP) modified Cu-MOF as precursor through high-temperature pyrolysis method. The phase structure, surface morphology and microstructure information of as-synthesized catalyst were systematically characterized by XRD, Raman, SEM, XPS and TEM. Norfloxacin (NOR) degradation in Cu@CN/air system showed Cu@CN3-600, prepared by using 0.3 g PVP as N source and pyrolysis temperature of 600 ℃, exhibited excellent catalytic activity and stability as well as universality in treating various organic wastewaters. The removal rate of NOR after 60 min was 96.05 % and meantime total organic carbon (TOC) decreased by 49.80 % under pH 4.0 and 1.2 g/L catalyst. After three cycles, it still maintained 81.53 % removal rate, owing to the protection effect of N doped carbon on active Cu component against its leaching during degradation. The reaction mechanism of Cu@CN3-600 activating O 2 for NOR degradation was deciphered by reactive oxygen species scavenging experiment, electron paramagnetic resonance (EPR) and density functional theory (DFT) calculation. Finally, four possible degradation pathways were proposed by identifying 16 intermediates through liquid chromatography-mass spectrometry (LC-MS) technology. This work can provide a guidance for designing highly efficient Cu-based molecular oxygen activation catalyst for wastewater abatement.
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PROCESS BIOCHEMISTRY
·
2024
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IF 3.7
Hongbo Suo,Xinzheng Liu,Shu Chen,Qi Li,Xiangnan Liu,Lili Xu
Biodiesel is more environmentally friendly compared to traditional petroleum diesel. The method of producing biodiesel catalyzed by lipases, as a green chemistry technology, can further reduce its negative impact on the environment. In this work, lipase immobilized on magnetic cellulose was embedded in Cu(PABA), and then the biocomposite (MCL@Cu(PABA)) was used for biodiesel production. The good biocompatibility and flexible skeleton structure of cellulose can buffer the compression effect on enzyme molecules during the formation of Metal-Organic Frameworks (MOFs), and the MOFs protective layer can reduce the damage caused by denaturants to enzyme molecules. The biocatalyst showed enhanced activity and stability with a lower deactivation constant ( K d ). Under the optimized reaction conditions, the biodiesel yield can reach 78.4 %. After reused for 7 times, the biocatalyst can still achieve a biodiesel yield of 58.8 %. Moreover, after stored for 30 days, the biodiesel yield can still reach 70.3 %. For all experimental yields, the standard deviation (SD) ranged from 2.4 % to 4.5 %. Secondary structure analysis showed that the rigid structure and active conformation of lipase was enhanced after Cu(PABA) encapsulation.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
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IF 8.1
Fan Feng,Haiyang He,Dan Liu,Siqing Liu,Jianjun Fang,Shuming Wen
This study presents an organic reagent, quercetin, as a flotation depressant used to effectively separate chalcopyrite and galena. Quercetin and O-isopropyl-N-ethyl thionocarbamate (IPETC) are used as depressants and collectors, respectively, and results of micro-flotation tests showed that quercetin can depress galena and has less effect on chalcopyrite. Tests of artificially mixed samples of the chalcopyrite and galena show that the separation effect of quercetin as a depressant is better than that of sodium sulfate and sodium silicate combined depressant, it is close to that of potassium bichromate as a depressant, that is, it has the potential to be a depressant to achieve selective separation of chalcopyrite and galena. The X-ray Photoelectron Spectroscopy and Fourier Transform Infrared Spectroscopy results demonstrate that quercetin can chemisorb with oxidized metal sites on minerals’ surfaces. Results of the contact angle, adsorption capacity, and Atomic Force Microscope show that quercetin has comparable adsorption amounts on both minerals’ surfaces, and can hinder the IPETC adsorption on the mineral surface, but the amount of IPETC adsorb on chalcopyrite is much higher than on galena surfaces. The differences in the adsorption of the collector on their surface are the main reason for realizing the separation of chalcopyrite from galena.
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