CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2026
·
IF 3.5
Xiaoxuan Guo,Jianan Li,Yin Wang,Yongning Chen,Yan Wang,Zhiqiang Fu,Wenbo Sun,Chong Peng
Pd-doped NiCo layered double hydroxide nanosheets were designed for efficient plastic upcycling. • Achieved 94.6% GA Faradaic efficiency with a 0.49 mmol cm -2 h -1 production rate. • Pulsed electrolysis enables dynamic interfacial regulation to mitigate deactivation. • Direct upcycling of PET waste into high-purity value-added GA was demonstrated. The massive accumulation of polyethylene terephthalate (PET) waste necessitates innovative upcycling strategies to recover chemical energy and promote a circular economy. Herein, we report a process intensification strategy for the selective electro-oxidation of PET-derived ethylene glycol (EG) into value-added glycolic acid (GA) using pulsed electrolysis (PE) on a Pd-incorporated NiCo layered double hydroxide (Pd-NiCo-LDH/NF) nanosheet electrocatalyst. Compared with conventional constant-potential electrolysis (CE), the PE mode achieves a superior Faradaic efficiency of 94.6% and a production rate of 0.49 mmol·cm –2 ·h –1 at 1.10 V vs. RHE, representing an 8.2-fold enhancement in yield. In-situ Fourier transform infrared (FTIR) spectroscopy and nuclear magnetic resonance (NMR) analysis were carried out to decipher the enhancement mechanism. Crucially, the practical scalability and industrial potential were demonstrated in a flow electrolyzer using real PET hydrolysates, achieving closed-loop plastic valorization. This work provides a universal paradigm for designing energy-efficient electrocatalytic systems through dynamic interfacial regulation for sustainable chemical production. Download: Download high-res image (177KB) Download: Download full-size image
✓ 已验证
DOI
高影响因子
Small
·
2025
·
IF 12.1
Furong Qiao,Qinghua Liu,Haonan Chen,Zhiwei Yang,Lu Jiang,Xinya Chen,Miao Ji,Yaning Liu,Xiao Huang,Gang Lu
Electroreduction of carbon dioxide (CO 2 ER) has emerged as a promising strategy for converting greenhouse gas carbon dioxide into value-added carbon-based products under mild conditions. Among the diverse products, the C 2 compounds, including ethylene and ethanol, are particularly attractive due to their high commercial value and widespread industrial applications. Therefore, it is highly promising to improve the Faradaic efficiency (FE) of C 2 products during CO 2 ER. Herein, cuprous oxide (Cu 2 O) particles are partially encapsulated with silica (SiO 2 ) for significant improvement in FE of C 2 products during CO 2 ER. Compared with pristine Cu 2 O and SiO 2 -fully encapsulated Cu 2 O, the SiO 2 -partially encapsulated Cu 2 O demonstrates an improved FE of C 2 products to ≈70.9 ± 3.1% in an H-type cell. This unique improvement in FE of C 2 can be attributed to the accumulated * CO intermediates and well modulated C–C coupling on a partially SiO 2 -encapsulated Cu-based catalyst. The optimized surface coverage of SiO 2 can not only modulate the electronic structure of Cu for an improved CO 2 ER (including C–C coupling) but also expose enough continuous Cu surface for the coupling of two C-containing intermediates. Therefore, the production of C 2 species can be significantly promoted. This work offers a valuable insight into the designing and development of highly selective CO 2 ER catalysts toward C 2 species.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
RESEARCH ON CHEMICAL INTERMEDIATES
·
2025
·
IF 3.5
Hu Yaping,Zhai Shasha,Guo Yaping,Dang Shan,Li Jing,Yang Miao
Electrochemical reduction reaction of CO 2 (CO 2 RR) to C 1 and C 2 products can be achieved on Cu-based electrocatalysts. C 2 products exhibit higher energy density and economic value compared to C 1 products, making them more desirable as reduction products. However, the production of C 2 products on pure Cu catalysts involves multi-step proton-coupled electron transfer and C–C coupling steps, which are kinetically slow and result in poor catalytic activity and selectivity for the products. The cavity nanocubes Cu 2 O(0.13-AA), Cu 2 O(0.10-AA) and Cu 2 O(0.15-AA) catalysts were synthesized via wet chemical reduction by adjusting the concentration of the reducing agent. The electrochemical pre-reduction method was used to obtain Cu 2 O/Cu(0.13-AA), Cu 2 O/Cu(0.10-AA) and Cu 2 O/Cu(0.15-AA) catalysts for CO 2 RR. Cu 2 O/Cu(0.13 M-AA) catalyst achieves the high Faradaic efficiency (FE) of 39.98% for C 2 H 4 and 54.76% for C 2 products (C 2 H 4 , C 2 H 6 , and C 2 H 5 OH), with significant inhibition of the hydrogen evolution reaction. In situ Raman experiments demonstrate that the cavity structure of the nanocubes enhances the local concentration of *CO intermediates, thereby promoting the C–C coupling process and improving the selectivity of CO 2 reduction to C 2 products.
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Xiuzheng Deng,Jiangchuan Liu,Jun Cai,Dan Wang,Huihui Mao,Changhai Liu,Zhongyu Li,Zhenhui Kang,Qian Liang
High production capacity of C 2 products from CO 2 photoreduction remains a significant challenge owing to the difficulty of C-C coupling and weak hydrogenation. Herein, a novel stepwise C-C coupling and hydrogenation mechanism is developed on multisite catalyst to enhance the performance of photocatalytic CO 2 reduction to C 2 products. The active Co cluster, carbon dots (CDs) and Cs 3 Bi 2 Br 9 quantum dots (QDs) are reinforced with robust carbon matrix, which allows to accelerate mass/electron transport and improve stability of catalytic sites, enabling a competitive C 2 H 4 evolution rate of 57.60 μmol g cat −1 h −1 with 67.70 % C 2 H 4 selectivity. In situ experiments coupled with theoretical calculations verify that Co and CDs capture photogenerated electrons from Cs 3 Bi 2 Br 9 to form key intermediate Co-*CO-*CO-CDs. After *CO-*CO coupling on Co site, the proximal CDs provide plenty of protons to conduct continuous hydrogenation toward coupling site until C 2 H 4 is formed. This study paves a novel pathway to regulate C-C coupling and hydrogenation for CO 2 conversion to C 2 hydrocarbons.
研究领域:
催化化学
·
环境科学
·
材料科学
·
物理化学
·
能源化学
·
纳米科技
✓ 已验证
产品关联
DOI
高影响因子
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
·
催化材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Shitao Han,Wei Xia,Shuaiqiang Jia,Jiapeng Jiao,Ting Yao,Xue Dong,Min Wang,Jianxin Zhai,Jiahao Yang,Yijun Xie,Xueqing Xing,Haihong Wu,Mingyuan He,Buxing Han
Electrochemical CO 2 reduction reaction (CO 2 RR) using renewable energy to produce valuable multicarbon (C 2+ ) products is a promising approach for carbon emission reduction. In this work, we propose a new strategy to enhance the formation of hydrogen-containing intermediates using the excellent abilities of proton transportation and electronic structure modification of phosphorus (P). To realize this, an in situ electrodeposition method was proposed to prepare P-doped Cu catalysts. It was found that the electrodeposition potential significantly impacts the structure and catalytic performance of P-Cu catalysts. Specifically, the catalyst obtained at − 0.5 V vs. Ag/AgCl exhibited exceptional performance for CO 2 RR towards C 2+ products, achieving a Faradaic efficiency (FE) of ∼ 80.2 % and a partial current density of 40.4 mA cm −2 in an H-type cell. Furthermore, the catalyst demonstrated stability for at least 12 h. Experimental and density functional theory (DFT) studies revealed that the free energy of the hydrogenated process could be significantly reduced by the excellent proton transport ability of P, and the interaction of Cu with the unpaired electrons of carbon could be improved, leading to excellent adsorption ability of Cu for the intermediates and high FE of C 2+ products.
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Kejing Wang,Yongjun Liu,Zhiwen Li,Nan Cui,Lei Sun,Wei Huang
The valence states of Cu site are regarded as an important factor affecting the performance of syngas to higher alcohols (C 2+ OH). Regrettably, the role of Cu 0 and Cu + in CO hydrogenation to higher alcohols remains controversial due to the complexity of the reaction. In this study, Cu 0 and Cu 2 O powders are directly added as the precursors to adjust the ratios of Cu + /(Cu 0 +Cu + ) and Cu particle sizes in CuZnAl catalysts by a complete liquid-phase (CLP) technology. The CAT-Cu 0 catalyst with higher Cu 0 content shows the highest CO conversion (>15%) ascribing to the biggest S Cu , but is also accompanied by the highest CO 2 selectivity (>40%), while the CAT-Cu + catalysts with higher Cu + content displays relative better C 2+ OH selectivity (>60%) and stability due to a higher probability of CO insertion. In-situ DRIFTS experiments reveal that a synergy between larger Cu particle sizes (30～40 nm) and surface Cu + sites, in which larger Cu sizes enhances the probability of bridge CO adsorption, thereby favoring the C–O bond dissociation for CH x formation. Meanwhile, Cu + active sites provide a higher probability for CO/CHO insertion to form CH 3 CHO*/CH 2 CO* intermediates. This study further deepens our understanding of the critical controlling factors for highly selective synthesis of C 2+ OH from syngas over Cu-based catalysts.
研究领域:
化学工程
·
催化
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
BIORESOURCE TECHNOLOGY
·
2022
·
IF 11.889
Xiaohong Hu,Haiyong Wang,Qiying Liu,Yuhe Liao,Chenguang Wang,Longlong Ma
Both alkaline organosolv and formaldehyde stabilization pretreatment can yield high-quality lignin by preventing condensation. For the hydrogenolysis of the pretreated solid residues , the highest yield of C2–C4 chemicals was 66.8% under alkaline organosolv pretreatment for 60 min. Specifically, the crimped fibers and residual lignin and hemicellulose increased the surface roughness of the residue by 40.6%, the crystallinity index decreased to 44.4%, and the crystal size was reduced to 2.15 nm, which in turn promoted hydrogenolysis of the residue. However, the increase of crystallinity and crystal size and the decrease in surface roughness of the formaldehyde stabilization pretreatment residue greatly hindered the conversion of polysaccharides. In addition, residual formaldehyde on the residue may also inhibit catalyst activity. Overall, this study provides novel perspectives on the full utilization of biomass, as well as new insights into the conversion of polysaccharides.
研究领域:
生物质能
·
催化化学
·
材料科学
✓ 已验证
DOI
PubMed
高影响因子
ChemistrySelect
·
2025
·Vol. 10
·期 33
·e03600
·
IF 2
Jiaqin Wang,Fang Li,Yasi Wang,Wei Huang
Graphical The Al-doped ZnO catalyst has a lower work function, which is conducive to promoting the dissociation of CH x O* to form CH x *; it also facilitates the generation of Zn x+ and oxygen vacancies, which further promotes the generation of C 2+ OH. The direct conversion of syngas into C 2+ OH has attracted significant attention as a potential pathway for energy conversion. However, this process typically requires the use of precious metals or the collaborative action of multi-component catalysts, making it relatively complex. In this paper, simple and economical Al-doped ZnO catalysts were employed for the synthesis of C 2+ OH. The results show that the work function, Zn x+, and the relative content of oxygen vacancies are linearly related to C 2+ OH/ROH. When the doping amount was 7 mol%, the catalyst had the highest C 2+ OH/ROH (82.6 wt%), corresponding to the lowest work function value, the highest Zn x+ content, and the relative content of oxygen vacancies. We reveal that the successful synthesis of C 2+ OH depends not only on the low work function of the Al-doped ZnO but also on the existence of the oxygen vacancies and Zn x+ sites. Specifically, the low work function induced by Al doping facilitates electron transfer in the reaction, facilitating the dissociation of CH x O* into CH x *. Meanwhile, the presence of oxygen vacancies enhances the dissociative adsorption capacity of CO and facilitates the formation of CH x * species. The Zn x+ sites serve as active centers for carbon chain growth, promoting C–C coupling through the insertion of CO or CH x O* into CH x *, thereby achieving chain elongation.
研究领域:
催化化学
·
材料科学
·
化学工程
·
能量转换
✓ 已验证
产品关联
DOI
高影响因子
Small Science
·
2025
·
IF 8.3
Muhammad Kashif Aslam,Iftikhar Hussain,Sidra Hameed,Liang Wang,Muhammad Ehtasham ul Haq,Ali H. Al-Marzouqi,Maowen Xu
This study investigates the synergistic interaction of CuO and SnO 2 in a heterostructure catalyst (CuO@SnO 2 ) for the conversion of C1 carbon dioxide (CO 2 ) reduction products to C2 products and its application in high-performance aqueous Zn-CO 2 batteries. This synergistic combination enhances the Faradaic efficiency (FE) for ethanol production from 12.5% to 41.8%, shifting the selectivity from C1 to C2 products. The flow-type aqueous Zn-CO 2 battery exhibits an ultrahigh power density of 6.5 mW cm −2 , demonstrates a high discharge voltage of 0.9 V, and maintains stable operation over 140 cycles, underscoring the catalyst's exceptional reversibility and durability. During battery discharge, the system achieves a FE of 36.86% for ethanol production. These results highlight the pivotal role of the CuO@SnO 2 synergy in optimizing CO 2 conversion efficiency while generating electrical energy. The findings advance the development of dual-function energy storage systems that integrate renewable electricity generation with sustainable CO 2 utilization, paving the way for industrial-scale applications.
研究领域:
电化学
·
能量存储
·
二氧化碳利用
·
催化
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 13.2
Xinya Chen,Chengcheng Zhu,Qinghua Liu,Yaning Liu,Miao Ji,Haonan Chen,Lu Jiang,Gang Lu
Electroreduction of carbon dioxide (CO 2 ) to valuable chemicals provides a promising solution to reducing CO 2 emissions and alleviating energy crisis. Coating or grafting catalyst with organic molecules or polymers could effectively improve the Faradaic efficiency (FE) of C 2 products in CO 2 electroreduction (CO 2 ER). However, to date, most efforts have focused on single-component coatings to enhance the FE of C 2 products in CO 2 ER. Herein, the surface of copper (Cu) catalyst is simultaneously coated with a thin layer composed of both small molecule of benzotriazole (BTA) and polymer of polyvinyl chloride (PVC). This BTA&PVC-coated Cu catalyst demonstrates a high FE of C 2 products up to 71.0 ± 5.6% in an H-type electrochemical cell, in contrast to the FE of ~36% for bare Cu. The improved CO 2 ER performance is attributed to the effective stabilization of key reaction intermediates and optimized electronic structure on Cu surface, facilitated by the synergistic effect of the simultaneously coated BTA&PVC film. In addition, the BTA molecules could be perfectly confined within PVC matrix, resulting in a high catalytic stability. In summary, this work provides an effective strategy to effectively improve the FE of C 2 products in CO 2 ER and this strategy could be easily migrated to many other catalytic systems.
✓ 已验证
产品关联
DOI
高影响因子
Journal of the American Chemical Society
·
2026
·
IF 16.6
Jundi Cheng,Biao Zhou,Hao Zhang,Xupeng Liu,Hao Zhang,Furong Guo,Xiaoyi Zhang,Yuqing Hu,Jun Lin,Hao Li,Lizhi Zhang
Electrochemical CO2 reduction to multicarbon (C2+) hydrocarbons offers a promising route for value-added fuels and chemical feedstocks, yet its selectivity is usually limited by the sluggish symmetric C–C coupling. Herein, we demonstrate the synthesis of phosphidated Cu–Ni–Cu triangular single-atom cones (Ni1PCu2) by decorating Cu nanowires with Ni single atoms and P. These Ni1PCu2 can deliver an impressive CO2-to-C2+ hydrocarbon (C2H4 43%, C2H6 48%) Faradaic efficiency of 91% under solar light at an ultralow bias of −0.3 VRHE, and a stable C2+ hydrocarbon production rate of 370 μmol h–1 cm–2 for 4 days at 100 mA cm–2, where the Cu nanowires harness solar light to generate plasmonic electrons for the CO2 activation and its subsequent conversion to *CO, while electronegative phosphidation induces the formation of Cu+ sites to well stabilize *CO across high coverages. Strategically positioned Ni single atoms generate and confine active hydrogen (•H) for efficient hydrogenation of adjacent Cu+–*CO into Cu+–*CHO. The resulting Cu+–*CHO displays a weakened C–O bond and enhanced C nucleophilicity, allowing for solar-powered asymmetric C–C coupling with neighboring *CO toward efficient and selective C2+ hydrocarbon synthesis.
✓ 已验证
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）