JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Bowen Wang,Lu Song,Chen Peng,Ximeng Lv,Gengfeng Zheng
The acidic CO 2 reduction reaction (CO 2 RR) offers a promising approach to mitigate CO 2 reactant loss and carbonate deposition, which are challenging issues in alkaline or neutral electrolytes. However, the hydrogen evolution reaction (HER) competes in the proton-rich environment near the catalyst surface as a side reaction, reducing the energy efficiency of generating multi-carbon (C 2+ ) products. In this work, we proposed a palladium (Pd) doping strategy in a copper (Cu)-based catalyst to stabilize polarized Cu 0 -Cu + sites, thus enhancing the C C coupling step during the CO 2 RR while suppressing HER. At an optimal doping ratio of 6%, the Pd dopants were well dispersed as single atoms without aggregation, allowing for the stabilization of subsurface oxygen (O Sub ), preserving the polarized Cu 0 -Cu + active sites, and reducing the energy barrier of C C coupling. The Pd-doped Cu/Cu 2 O catalyst exhibited a peak Faradaic efficiency (FE) of 64.0% for C 2+ products with a corresponding C 2+ partial current density of 407.1 mA∙cm −2 at −2.18 V versus a reversible hydrogen electrode, a high CO 2 single-pass conversion efficiency (SPCE) of 73.2%, as well as a high electrochemical stability of ∼ 150 h at industrially relevant current densities, thus suggesting a potential approach for tuning the electrocatalytic CO 2 performances in acidic environments with higher carbon conversion efficiencies.
研究领域:
电化学
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催化材料科学
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高影响因子
Nanomaterials
·
2025
·Vol. 15
·期 2
·105
·
IF 4.3
Jiuyu Chen,Chensheng Gao,Jingwen Chen,Fei Liu,Zhiwen Liu
The development of copper-based materials with a high efficiency and low cost is desirable for use in iodine (I2) remediation. Herein, Cu0-nanoparticles-functionalized, ZIF-8 (Zeolite Imidazole Framework-8)-derived, nitrogen-doped carbon composites (Cu@Zn-NC) were synthesized by ball milling and pyrolysis processes. The as-prepared composites were characterized using SEM, BET, XRD, XPS, and FT-IR analyses. The results showed that the morphology of ZIF-8 changed from a leaf-like structure into an irregular structure after the introduction of a copper salt and carbonization. The copper in the pyrolysis samples was mainly in the form of Cu0particles. The presence of an appropriate amount of Cu0particles could increase the specific surface area of Cu@Zn-NC. The subsequent batch adsorption results demonstrated that the as-fabricated composites showed high I2adsorption amounts (1204.9 mg/g) and relatively fast dynamics in an iodine–cyclohexane solution when the Cu content was 30% and the pyrolysis temperature was 600 °C, outperforming the other Cu-based materials. The isothermal adsorption followed both Langmuir and Dubinin–Radushkevich isotherm models, while the kinetics of I2adsorption followed a pseudo-second-order kinetic model. The activation energy (Eα) of the adsorbent was determined to be 47.2 kJ/mol, according to the Arrhenius equation. According to the experimental and DFT analyses, I2-Zn interactions and I2-Cu0chemisorption jointly promoted the elimination of iodine. In general, this study provided an operative adsorbent for the highly effective capture of iodine in solution, which might be worth applying on a large scale.
研究领域:
环境科学
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材料科学
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Kai An,Hongyan Jia,Ruobing Cheng,Yong Guo,Xiaohui Liu,Yanqin Wang
Pt-based bimetallic catalysts have gained more and more attention in propane dehydrogenation (PDH), but still suffer from the high cost and poor stability. In this work, a PtCu@S-1 catalyst with an extremely low loading of Pt (0.047 wt%) is prepared by in-situ hydrothermal synthesis and employed in PDH. An excellent productivity (propylene yield: 471.8 molC 3 H 8 ⋅ g Pt -1 ⋅ h −1 ) is achieved at 600 °C with a weight hour space velocity of 25.80 h −1 . After 50 h of reaction at 600 ℃, 0.047Pt0.19Cu@S-1 catalyst still remains sinter-free, with a deactivation rate of only 0.006 h −1 . Various characterizations show that Cu 0 co-existed with Pt 0 in PtCu@S-1 catalyst plays an important role, greatly improved catalyst reactivity and stability. At high weight hour space velocity (44.5 h −1 ), the propylene productivity can reach 1056.4 molC 3 H 8 ⋅ g Pt -1 ⋅ h −1 . This work provides a new way for the design of extremely low Pt-loaded PDH catalysts with excellent performance at high temperatures.
研究领域:
催化化学
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材料科学
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高影响因子
ACS Sustainable Chemistry & Engineering
·
2026
·
IF 7.6
Jiahui Zhou,Ziyi Zhang,Chenghao Jin,ShanShan Tong,Yunteng Qu
Electrochemical CO2 reduction reaction (CO2RR) to diverse high-value chemicals represents a promising carbon mitigation strategy, yet precisely controlling product selectivity remains a considerable challenge. Herein, we report a size-dependent Cu/CN catalyst for modulating the selectivity of CO2RR. Specifically, small Cu NPs on CN (∼5 nm, S–Cu/CN) achieved a 76.2% C2+ product selectivity at 0.6 A cm–2, while the large one (∼50 nm, L-Cu/CN) reached a 67.5% CH4 selectivity at 0.6 A cm–2. Physical characterizations revealed that S–Cu/CN displays partial Cu+ sites, whereas L-Cu/CN higher Cu+ content. Mechanism analysis revealed a balanced Cu0/Cu+ ratio in S–Cu/CN promotes C–C coupling at Cu+ sites to form C2+ products. Conversely, higher Cu+ content in L-Cu/CN decreased the *CO coverage and improved H2O dissociation, steering continuous hydrogenation toward CH4 generation. This work offers a novel strategy to design high-efficiency CO2RR electrocatalysts toward desired products.
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高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2026
·
IF 5.1
Jiuyu Chen,Zhiwen Liu,Zenghui Liu,Hao Wu,Chensheng Gao,Jiaqi Shi,Dingming Xue
Radioactive iodine ( 131 I and 129 I) produced by the development of nuclear energy poses a long-term threat to ecology and health. In this study, a series of Cu@Mn x Cu 10-x -C materials were synthesized using Mn x Cu 10-x -BTC as the precursor, followed by surface grinding with external copper salts and subsequent pyrolysis. The material achieved a uniform dispersion of high-density Cu 0 sites on the Mn-Cu carbon framework. The optimal material Cu@Mn 3 Cu 7 -C had saturated adsorption capacities of 346.6 mg/g and 1555.3 mg/g for iodide (I − ) and iodine (I 2 ) respectively, further improving under acidic and oxygen-rich conditions. In addition, it could maintain excellent I − adsorption performance in the presence of highly competitive anions, in actual water samples, and after high-dose γ-irradiation. Mechanism studies demonstrated that Cu 0 , as the reaction center, dominated the oxidation-adsorption of I − and the reduction and fixation of I 2 , while triiodide (I 3 − ) could be effectively eliminated through the [Cu → I 3 ] charge transfer complexation or disproportionation pathway. The Mn species cooperated with the Cu site through valence modulation and electron transfer. This study provides a material system and theoretical basis for the efficient removal of multiple iodine species in complex water bodies with high capacity, fast kinetics and good environmental adaptability.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Man Zhao,Wei Wen,Chunmei Liu,Qinyun Yan,Shuai He,He Xiao,Li Zhang,Junming Zhang,Xiaofeng Gao,Jianfeng Jia
The electrochemical CO 2 reduction reaction (CO 2 RR) to multi‑carbon products offers a promising route for sustainable fuel production, yet achieving high selectivity remains challenging due to the complex interplay between catalyst structure and reaction pathways. Here, we report a rational design of Cu-Cu 2 O/graphene (Cu/G) composites with tunable Cu + /Cu 0 ratios via electrolyte-mediated electrochemical synthesis. By varying tetraalkylammonium/phosphonium electrolytes (TBABF 4 , TBAPF 6 , TBACF 3 SO 3 , TBPBF 4 ), we precisely control Cu oxidation states, as validated by the results of X-ray absorption fine structure (XAFS), X-ray diffraction (XRD), and high-resolution transmission electron microscope (HRTEM). In-situ Fourier transform infrared (In-situ FTIR) spectra and in-situ Raman spectra indicate Cu + -rich surfaces (Cu/G-TBABF 4 ) favor the production of formate via O-bound intermediates, while Cu 0 -dominated interfaces (Cu/G-TBAPF 6 ) promote the formation of CO through C-bound pathways. Mixed Cu + /Cu 0 systems (Cu/G-TBACF 3 SO 3 , Cu/G-TBPBF 4 ) enable C C coupling, with ethylene (FE = 28 %) and ethanol (FE = 30.2 %) selectivity governed by the Cu + /Cu 0 balance. Ultraviolet photoelectron spectroscopy (UPS) results reveal that lower work functions enhance *CO coverage and stabilize C 2+ intermediates, elucidating the electronic structure-activity relationship. This work demonstrates electrolyte-mediated oxidation state engineering as a versatile strategy to steer CO 2 RR pathways, offering a generalizable approach for designing multi-valent electrocatalysts with tailored selectivity.
研究领域:
电催化
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材料科学
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能量转换
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表面化学
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光谱学
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PubMed
高影响因子
ACS Sustainable Chemistry & Engineering
·
2025
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IF 7.3
Kai Zhu,Zihan Lin,Xinyi Bai,Fangfang Chang,Qing Zhang,Xiaolei Wang,Zhengyu Bai
Electrocatalytic reduction reaction of CO2 (CO2RR) into value-added multicarbon (C2+) products represents a sustainable strategy for mitigating greenhouse gas emissions and enhancing the production of high-value chemicals. Cu-based catalysts are optimal for the CO2RR, facilitating the generation of C2+ products such as ethanol, which have significant industrial applications. However, converting CO2 to C2+ products remains a great challenge, necessitating the simultaneous achievement of high current density, Faradaic efficiency (FE), and operational stability for industrial-scale implementation. Herein, we prepared Cu/Cu2O catalysts with diverse morphologies and the ratio of the Cu+/Cu interface, which was rectified by regulating the interactions between the active interface and the intermediate (*CO). The electrochemical analysis demonstrated that reconstructed Cu/Cu2O nanodendrites with dominant grain boundaries exhibited remarkable performance in generating C2+ products, achieving a Faradaic efficiency (FE) of 71.8%, including 49.7% FE of ethanol and a substantial partial current density of 390.0 mA cm–2 within the flow cell. In situ spectroscopy characterization and theoretical calculations revealed that the increased ethanol selectivity originated from the rectification of the Cu/Cu2O interface by the *CO intermediate, which accelerated H2O dissociation, reduced the free energy for *CO hydrogenation to *COH, and facilitated asymmetric *CO-*COH coupling to preferentially reduce CO2 to ethanol. This study provides profound insights into the C–C coupling pathways and sheds light on the rational design of ethanol-oriented electrocatalysts, contributing to sustainable chemical synthesis and energy utilization.
研究领域:
电催化
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能量转换
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材料科学
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环境化学
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化学工程
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高影响因子
Desalination and Water Treatment
·
2026
·
IF 3.4
Yantao Zhu,Jianping Sun,Ying Xie,Qiyu Liu,Fu Zhu,Yetong Chen,Zeyu Wang,Manni Li,Hassaan Ahmad Butt,Huizhong Chi
Cu 0 - activated peroxymonosulfate (PMS) is a promising advanced oxidation process for the removal of pharmaceuticals and personal care products, yet its performance is often limited by inefficient Cu(II)/Cu(I) redox cycling as well as the low steady-state availability of reactive copper species. Here, we constructed a Cu 0 /HA/NCP/PMS system by integrating hydroxylamine as a reductant and neocuproine as a Cu(I) - complexing ligand to intensify naproxen degradation and investigate the underlying activation pathway. Under typical conditions, the synergistic combination of HA and NCP caused NPX removal to enable 98.57% within 6 min. This is significantly higher than those in Cu 0 /PMS, Cu 0 /NCP/PMS, and Cu 0 /HA/PMS. The system maintained high efficiency across pH 3.0 ~ 7.0. Scavenging tests and nitrobenzene probing indicated that ⋅ O H / S O 4 ⋅ − pathways were not dominant, whereas benzoic acid caused only moderate inhibition, collectively supporting a non-radical pathway. Spectroscopic and LC-MS evidence revealed a ligand-stabilized high-valent copper oxidant, with characteristic absorption at 358 nm and a signal at m/z 479 assigned to [Cu(III) - (NCP) 2 ] 3+ . This work provides a mechanistically grounded “reduction and complexation” strategy to overcome Cu - based persulfate activation bottlenecks and achieve rapid, pH - resilient degradation of NPX.
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高影响因子
Nature Communications
·
2023
·Vol. 14
·期 1
·1-12
·
IF 16.6
Meng Hao,Yang Yusen,Shen Tianyao,Yin Zhiming,Wang Lei,Liu Wei,Yin Pan,Ren Zhen,Zheng Lirong,Zhang Jian,Xiao Feng-Shou,Wei Min
Copper-based catalysts serve as the predominant methanol steam reforming material although several fundamental issues remain ambiguous such as the identity of active center and the aspects of reaction mechanism. Herein, we prepare Cu/Cu(Al)O x catalysts with amorphous alumina-stabilized Cu 2 O adjoining Cu nanoparticle to provide Cu 0 −Cu + sites. The optimized catalyst exhibits 99.5% CH 3 OH conversion with a corresponding H 2 production rate of 110.8 μmol s −1 g cat −1 with stability over 300 h at 240 °C. A binary function correlation between the CH 3 OH reaction rate and surface concentrations of Cu 0 and Cu + is established based on kinetic studies. Intrinsic active sites in the catalyst are investigated with in situ spectroscopy characterization and theoretical calculations. Namely, we find that important oxygen-containing intermediates (CH 3 O* and HCOO*) adsorb at Cu 0 −Cu + sites with a moderate adsorption strength, which promotes electron transfer from the catalyst to surface species and significantly reduces the reaction barrier of the C−H bond cleavage in CH 3 O* and HCOO* intermediates.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Huaiwei Zhang,Liang Bao,Qingwei Zhou,Ying Pan,Jingyuan Ge,Jia Du
The photocatalytic performance of ceria-based materials can be tuned by adjusting the surface structures with decorating the transition-metal, which are considered as the important active sites. Herein, cuprous oxide-metallic copper composite - doped ceria nanorods were assembled through a simple hydrothermal reduction method. The photocatalytic ammonia synthesis rates exhibit an inverted “V-shaped” trend with increasing Cu 0 /Cu x O mole ratio. The best ammonia production rate, approximately 900 or 521 µmol·g cal −1 ·h −1 under full-spectra or visible light , can be achieved when the Cu 0 /Cu x O ratio is approximately 0.16, and this value is 8 times greater than that of the original sample. The absorption edge of the as-prepared samples shifted towards visible wavelengths, and they also had appropriate ammonia synthesis levels. This research provides a strategy for designing noble metal-free photocatalysts through introducing the metal/metallic oxide composites to the catalysts.
研究领域:
材料科学
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催化化学
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PubMed
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-11
·
IF 15.7
Lu Yuxuan,Yue Feng,Liu Tianyang,Huang Yu-Cheng,Fu Feng,Jing Yu,Yang Hengquan,Yang Chunming
The synergistic Cu 0 -Cu + sites is regarded as the active species towards NH 3 synthesis from the nitrate electrochemical reduction reaction (NO 3 - RR) process. However, the mechanistic understanding and the roles of Cu 0 and Cu + remain exclusive. The big obstacle is that it is challenging to effectively regulate the interfacial motifs of Cu 0 -Cu + sites. In this paper, we describe the tunable construction of Cu 0 -Cu + interfacial structure by modulating the size-effect of Cu 2 O nanocube electrocatalysts to NO 3 - RR performance. We elucidate the formation mechanism of Cu 0 -Cu + motifs by correlating the macroscopic particle size with the microscopic coordinated structure properties, and identify the synergistic effect of Cu 0 -Cu + motifs on NO 3 - RR. Based on the rational design of Cu 0 -Cu + interfacial electrocatalyst, we develop an efficient paired-electrolysis system to simultaneously achieve the efficient production of NH 3 and 2,5-furandicarboxylic acid at an industrially relevant current densities (2 A cm −2 ), while maintaining high Faradaic efficiencies, high yield rates, and long-term operational stability in a 100 cm 2 electrolyzers, indicating promising practical applications.
研究领域:
材料科学
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电化学
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环境科学
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PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Yanjing Liu,Ruitao Wang,Shuhong Liu,Yunsong Xu,Zhirong Zhang,Ying Song,Zhongping Yao
The Fenton-like activated molecular oxygen technology demonstrates significant potential in the treatment of refractory organic pollutants in wastewater, offering promising development prospects. We prepared a N -doped C -coated copper-based catalyst Cu 0 /NC3-600 through the pyrolysis of Mel-modified Cu-based metal–organic framework (MOF). The results indicate that the degradation of 20 mg/L norfloxacin (NOR) was achieved using 1.0 g/L Cu 0 /NC3-600 across a wide pH range, with a removal rate exceeding 95 % and total organic carbon (TOC) removals approaching 70 % after 60 min at pH 5–11. The nitrogen doping enhances the electronic structure of the carbon material, facilitating the adsorption of molecular oxygen. Additionally, the formed carbon layer effectively prevent copper leaching,contributing to increased stability to a certain extent. Subsequently, we propose the catalytic reaction mechanism for the Cu 0 /NC/air system. Under acidic conditions, Cu 0 /NC3-600 activates molecular oxygen to produce the •O 2 – , which serves as the primary active species for NOR degradation. While in alkaline conditions, the high-valent copper species Cu 3+ is generated in conjunction with •O 2 – , both working simultaneously for NOR degradation. Furthermore, based on the LC-MS results, we deduced four possible degradation pathways. This work offers a novel perspective on expanding the pH range of copper-based catalysts with excellent ability to activate molecular oxygen for environmental water treatment.
研究领域:
环境科学
·
材料科学
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高影响因子
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