ACS Applied Nano Materials
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2025
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IF 5.5
Yilin Wang,Yuping Chen,Shuang Yao,Furong Zhao,Linxiu Dai,Xian Yang,Changhua An
Electrochemical CO2 energization represents a promising strategy to mitigate its emission and promote resourceful utilization. The production of alcohols offers a sustainable pathway for converting CO2 into value-added chemicals, which is often hindered by low selectivity and high overpotential. In this work, a class of ultrasmall La2O3 nanoparticle-modified Cu2O-based catalyst has been synthesized in situ on a copper foam substrate through a simple hydrothermal method. The optimized catalyst demonstrated a high ethanol Faradaic efficiency of 51.7% at −1.0 V versus the reversible hydrogen electrode (RHE); simultaneously, syngas (CO/H2) was generated with Faradaic efficiencies of 28.27% for CO and 4.8% for H2. This product distribution characteristic enables efficient separation and utilization of both liquid (ethanol) and gaseous (syngas) products. This study highlights the pivotal role of rare earth elements in enhancing CO2RR efficiency by stabilizing reaction intermediates for facilitating C–C coupling. Furthermore, it presents a scalable and cost-effective approach for CO2 energization, paving the way for sustainable green energy production and carbon resource management.
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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Xueli Zhou,Qingyuan Song,Jing Chen,Chunhong Chen,Yuhuan Chen,Fang Yang
Blended amine mixtures show great superiorities in CO 2 absorption capacity and energy efficiency. This work focuses on the absorption-desorption performance of CO 2 capture by mixed amine solutions based on N, N-diethylethanolamine (DEEA). Four bi-solvent blends consisting of DEEA and 2-amino-2-methyl-1-propanol (AMP)/1-(2-hydroxyethyl) piperazine (HEPZ)/1-ethylpiperazine (N-1EPZ)/piperazine (PZ) are studied. The CO 2 loading, absorption rate, average absorption rate, desorption loading, average desorption rate, desorption efficiency and relative heat duty are comprehensively investigated to explore the performance of blended absorbents. Experimental investigations on concentration reveal that blended 20 wt% DEEA +10 wt% PZ solution demonstrates outstanding CO 2 equilibrium loading, absorption rate and average absorption rate, and 20 wt% DEEA +10 wt% AMP system exhibits excellent CO 2 desorption performance. The average desorption rate, desorption loading and desorption efficiency increase by 91.47 %, 91.09 % and 122.30 % in contrast to the single amine solution, i.e. aqueous 30 wt% MEA, respectively. Therefore, mixed amine solutions can largely reduce the energy requirement for CO 2 regeneration, which confirms blended amine mixtures are energy-efficient. Additionally, 13 C NMR and FT-IR spectra are conducted to elucidate the mechanism of DEEA-based mixed amine systems for CO 2 capture.
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ADVANCED MATERIALS
·
2025
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IF 26.8
Yuchun Liu,Tianqi Liu,Xinyun Wang,Jing Zhang,Xingwu Zhai,Tianchen Wei,Qianqi Shi,Chengjie Lu,Huan Yan,Yujian Xia,Weiren Cheng,Min Zhou
Li-CO₂ batteries promise ultrahigh theoretical energy densities but face efficiency limitations owing to the sluggish decomposition of stable Li 2 CO 3 . Redirecting the redox pathway toward Li 2 C 2 O 4 overcomes this challenge, but its metastability leads to facile conversion to Li 2 CO 3 during discharge. Herein, subsurface electronic confinement is engineered in Mo-based catalysts, leveraging electron-deficient boron (B) as electron traps in the subsurface atomic layers to tailor their interfacial electronic landscapes. This design elevates the Mo d-band and intensifies the hybridization between the Mo d-orbitals and O p-orbitals of oxalate. Strengthening the Mo-O interaction stabilizes Li 2 C 2 O 4 against decomposition. The highly reversible and stable redox chemistry enabled by MoB results in an exceptional cycling stability and energy efficiency across a wide temperature range, with an expanded practical viability. At 70 µA cm −2 , the MoB-based battery is cycled for >1400 h with a high energy efficiency of >85%. The energy efficiency even remains at >90% for ≈150 h at a high temperature (90 °C). This study pioneers a material design framework for use in stabilizing metastable products within Li-CO 2 batteries, advancing their applicabilities in extreme environments, such as deep-earth exploration, by revealing the role of subsurface charge redistribution in steering reaction pathways.
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ACS Sustainable Chemistry & Engineering
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2025
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IF 7.3
Xiarui Yan,Junsheng Chen,Zhaorui Kong,Xinyi Wan,Youmin Hou,Bin Hua
Research on CO2 hydrogenation catalysts, particularly In2O3-based materials, is crucial for developing sustainable CO2 utilization and chemical production technologies, contributing to a cleaner future. We address the critical challenge of efficient and stable CO2 conversion by developing a novel Zr-doping strategy to enhance In2O3 catalyst performance for CO2 hydrogenation to methanol. Our key contribution is identifying the nanoscale confinement effect as crucial for optimizing both the activity and stability of In2O3 catalysts. By leveraging this nanoscale confinement effect, we have precisely controlled the size, dispersion, and reducibility of In2O3 nanoparticles, resulting in the formation and stabilization of highly active In2O3–x with oxygen vacancies. This confinement also effectively suppresses In0 migration and sintering, dramatically improving catalyst stability. The resulting Zr-doped catalysts exhibit significantly higher activity and stability compared to the undoped In2O3/ZrO2 catalyst, achieving a remarkable space-time yield of 4.708 gMeOH gIn–1 h–1 and demonstrating durability under industrially relevant conditions. This discovery offers a promising new direction for the rational design of high-performance CO2 hydrogenation catalysts and lays the foundation for future advances in sustainable catalysis.
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ACTA PHYSICO-CHIMICA SINICA
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2025
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IF 13.5
Qinhui Guan,Yuhao Guo,Na Li,Jing Li,Tingjiang Yan
In the realm of photocatalytic CO 2 hydrogenation, the adsorption-desorption behaviors and dynamics of photogenerated carriers are pivotal determinants of the kinetic processes and overall efficiency of photocatalytic reactions. Herein, 5A molecular sieve-functionalized In 2 O 3 composites (denoted as IO@5A- x wt%) were fabricated through a facile impregnation-calcination method. Among them, the IO@5A-5wt% composite, with the optimized loading amount of 5A molecular sieves, showcases outstanding performance in photocatalytic conversion of CO 2 to CO, achieving a CO production rate of 2610.55 μmol·g −1 ·h −1 , which is 19 times higher than that of pristine In 2 O 3 . Moreover, the IO@5A-5wt% composite maintains acceptable catalytic stability after a prolonged experiment lasting 45 hours and total of 108 cycles. A comprehensive series of characterization techniques and performance evaluations reveal that the incorporation of 5A molecular sieves significantly modulates the adsorption-desorption behavior and hole dynamics during photocatalytic reactions. The multi-channel architecture of 5A molecular sieves, featuring suitable pore sizes, effectively enhances CO 2 adsorption. Meanwhile, the surface hydroxyl groups of 5A molecular sieves facilitate the transfer of photogenerated holes, thereby suppressing the recombination of photogenerated carriers. Additionally, the reaction product H 2 O desorbs more readily from the catalyst surface. These synergistic effects collectively constitute the key mechanism underlying the enhanced photocatalytic performance of the IO@5A-5wt% composite.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Xiaopeng Li,Haichao Wang,Qingxiang Ma,Jucang Ke,Xiuyun Jiang,Caixia Zhu,Linlin Zhao,Ao Zhang,Hao Chen,Yao Deng,Xinhua Gao,Guangbo Liu,Tian-Sheng Zhao,Noritatsu Tsubaki
The conversion of CO 2 into ethanol with value-added still exists challenge, especially the CO 2 hydrogenation over Co-based catalysts is still C1 product dominated by CH 4 . Here, we report a xNa-CoMnO catalyst to promoting ethanol synthesis from CO 2 hydrogenation. The experimental results indicated that there was almost no adsorption and conversion of CO 2 on pure Co 0 , and the CO 2 hydrogenation production of the CoMnO catalyst prepared by adding Mn was mainly CH 4 . The loading of Na not only increased the concentration of oxygen defects on the CoMnO catalyst, but also improved the strength of the Co-O in the CoMnO catalyst, which was able to adsorb effectively the undissociated *CO in the reaction process, and promote the C-C coupling between the *CO and the generated *CH x , promoted the synthesis of ethanol. Under optimized reaction conditions (240 °C, 3.0 MPa, GHSV = 1200 mL/g/h), the 2Na-CoMnO catalyst showed ethanol selectivity of 18.89 % and space-time yield of ethanol of 1.27 mmol/g/h, which exceeded most of the reported results. More importantly, beyond delivering an excellent-performance catalytic system, this study also provides fundamental insights for the rational design of Co-based catalysts for selective CO 2 -to-ethanol conversion.
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ACS Nano
·
2022
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IF 18.027
Peng Wang,Tan Li,Qiqi Wu,Ruian Du,Qinghua Zhang,Wei-Hsiang Huang,Chi-Liang Chen,Yan Fan,Haonan Chen,Yanyan Jia,Sheng Dai,Yongcai Qiu,Keyou Yan,Yuanyuan Meng,Geoffrey I. N. Waterhouse,Lin Gu,Yun Zhao,Wei-Wei Zhao,Guangxu Chen
In certain metalloenzymes, multimetal centers with appropriate primary/secondary coordination environments allow carbon–carbon coupling reactions to occur efficiently and with high selectivity. This same function is seldom realized in molecular electrocatalysts. Herein we synthesized rod-shaped nanocatalysts with multiple copper centers through the molecular assembly of a triphenylphosphine copper complex (CuPPh). The assembled molecular CuPPh catalyst demonstrated excellent electrochemical CO2 fixation performance in aqueous solution, yielding high-value C2+ hydrocarbons (ethene) and oxygenates (ethanol) as the main products. Using density functional theory (DFT) calculations, in situ X-ray absorption spectroscopy (XAS) and quasi-in situ X-ray photoelectron spectroscopy (XPS), and reaction intermediate capture, we established that the excellent catalytic performance originated from the large number of double copper centers in the rod-shaped assemblies. Cu–Cu distances in the absence of CO2 were as long as 7.9 Å, decreasing substantially after binding CO2 molecules indicating dynamic and cooperative function. The double copper centers were shown to promote carbon–carbon coupling via a CO2 transfer-coupling mechanism involving an oxalate (OOC–COO) intermediate, allowing the efficient production of C2+ products. The assembled CuPPh nanorods showed high activity, excellent stability, and a high Faradaic efficiency (FE) to C2+ products (65.4%), with performance comparable to state-of-the-art copper oxide-based catalysts. To our knowledge, our findings demonstrate that harnessing metalloenzyme-like properties in molecularly assembled catalysts can greatly improve the selectivity of CO2RR, promoting the rational design of improved CO2 reduction catalysts.
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Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Shuangjiang Li,Yi Liu,Lan Shi,Tianding Hu,Mengrui Li,Churu Zhang,Shaoyun Shan,Yunfei Zhi
A Salen-functionalized ionic polymer (Zn-Salen-IP) was synthesized through a metal-assisted method. The structure and microstructure were characterized by using different characterization methods. Subsequently, the cycloaddition of CO 2 with epoxide was used to investigate the catalytic activity of Zn-Salen-IP. The relationship between the types of ions within Zn-Salen-IP and its catalytic performance was thoroughly explored. Single-factor investigations were used to determine the optimal reaction conditions for catalytic CO 2 cycloaddition used Zn-Salen-IP. The universality and recyclability of Zn-Salen-IP were systematically studied under the optimized conditions. Finally, Density functional theory calculations were employed to research the mechanism and pathway of the CO 2 cycloaddition reaction catalyzed by Zn-Salen-IP with dual functional active sites. This provided a deep understanding for the rate-determining step and the influence of the nucleophilicity of the halogen anion in cycloaddition reaction of CO 2 and epoxide.
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Catalysis Science & Technology
·
2024
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IF 4.4
Shuai Yan,Yuting Wang,Guangyao Chen,Wanli Ma,Yingquan Chen,Xianhua Wang,Kuo Zeng,Yonggang Yao,Hongqi Sun,Haiping Yang,Hanping Chen
Transition metals doping for Fe-based catalysts has been demonstrated in promoting the activity and regulating the selectivity in both reverse water gas shift reaction and Fischer-Tropsch synthesis. However, there are few studies that concern their catalytic performances tailored by these promoters under photothermal conditions. In this study, a series of typical MFeOx (M = Mn, Co, Cu, Zn) catalysts were synthesized with a facile co-precipitation method and their photothermal CO2 hydrogenation properties were evaluated. The results showed that the doping of Co, Cu, and Zn enhanced the activity and regulated the selectivity of Fe-based catalysts, e.g., CoFe achieving a C2+ yield of 1.73 mmol·h-1·g-1 while ZnFe almost doubling the CO2 conversion under irradiations. Mechanistic studies suggest that Co and Cu facilitated the reduction of Fe species, resulting in favorable CO2 and H2 activation. At last, a light-induced direct CO2 dissociation pathway was proposed with in situ EPR and DRIFTS characterization and analysis of the undoped Fe and ZnFe catalyst. This study provides a novel perspective on transition metal promoters for photothermal CO2 hydrogenation over Fe-based catalysts.
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ACS Nano
·
2024
·
IF 15.8
Xue Tian,Huan Liu,Bin Cao,Peng Zhang,Yanze Li,Yanchao Ou,Haonan Cui,Mengyao Xu,Bin Xu
MXenes are promising cathodes for Li–CO2 batteries owing to their high electrical conductivity and efficient CO2 activation function. However, the effects of adsorption and electronic structures of MXene on the full life cycle of Li–CO2 batteries have been rarely investigated. Here, we employ a coregulation approach to enhance the adsorption–decomposition of lithium carbonate (Li2CO3) by introducing Zn and Cl surface groups onto the Ti3C2 MXene (Zn–Ti3C2Cl2) catalyst. The incorporation of Cl surface groups enhances Li2CO3 adsorption on the MXene catalyst surface, resulting in the formation of small-sized and uniform Li2CO3. Additionally, the introduction of Zn shifts the d-band centers of titanium and promotes CO2 evolution reaction (CO2ER) activity, thereby facilitating the decomposition of discharge products. As a result, the Li–CO2 battery based on the Zn–Ti3C2Cl2 catalyst exhibits an ultralow overpotential (0.72 V) at 200 mA g–1 and stable cycling for up to 1500 h. This work validates the efficacy of promoting reversibility in Li–CO2 batteries by adjusting the adsorption-decomposition process.
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ACS Applied Nano Materials
·
2025
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IF 5.5
Jin Li,Zhujun Chen,Xin Li,Bingshuang Li,Pengxuan Wu,Xiaoxi Huang
Indium sulfide-based electrocatalysts often suffer from the reduction of In3+ to In0 species in the electrocatalytic CO2 reduction reaction (CO2RR), and this dynamic transformation leads to undesired hydrogen evolution reaction. Promoting the stability of high-valent In3+ species under operating conditions is a challenging but important task for maintaining their excellent electrocatalytic activity. In this work, In2S3 electrocatalysts with controllable crystallinity are synthesized by a hydrothermal reaction at a tunable temperature. The low-crystalline In2S3-1 exhibits more abundant defective and amorphous/crystalline interface structures compared with the high-crystalline ones, thus endowing the low-crystalline In2S3-1 with a higher formate faradaic efficiency (FEformate) of 91.6% at −1.45 V vs RHE in the H-type cell compared with the high-crystalline In2S3-3 (FEformate = 79.3%). This improved electrocatalytic activity can be attributed to its abundant defect structures and amorphous/crystalline interface structures with robustly high-valent In3+ species under the operating conditions. In situ attenuated total reflectance Fourier transform infrared (ATR-FTIR) spectroscopy results reveal the *OCHO reaction pathway. Density functional theory (DFT) calculations indicate that defective structures, such as sulfur vacancies, play an important role in lowering the energy barrier for the key intermediate *OCHO formation. This work provides important insight into defect engineering to promote CO2RR.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
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IF 20.2
Yanqiu Wang,Ying Zhou,Xinxin Zhang,Mingrui Wang,Tangkang Liu,Jinxing Wei,Guanghui Zhang,Xinlin Hong,Guoliang Liu
Direct CO 2 hydrogenation to higher alcohols (HA) is a promising route for high-value utilization of waste CO 2 , but developing active and stable catalysts remains a grand challenge. For this reaction, constructing multifunctional interfaces as active sites is required to fulfill controllable C-C coupling of alkyl and CO*/CH x O* species. Herein, we report a PdFe catalyst with abundant PdFe alloy-Fe 5 C 2 interfaces via a PdFe alloy induced FeO x carbidization process, which can achieve HA yield of 86.5 mg g cat −1 h −1 with 26.5% selectivity at 300 ºC, 5 MPa, and 6000 mL g cat −1 h −1 . The accelerated deactivation test unveils the PdFe catalyst exhibits better durability than the widely studied CuFe based catalysts against harsh conditions. Multiple in-situ characterization results unveil a synergetic mechanism for HA synthesis at the PdFe alloy-Fe 5 C 2 interfaces, where PdFe alloy is responsible for CO formation and non-dissociative activation, while Fe 5 C 2 phase promotes CO dissociation and chain propagation.
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