APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
·
IF 21.1
Long Cheng,Rong Wang,Ya Wang,Xingxia Yang,Yanxi Deng,Junhua Li
Formic acid (HCOOH) production from direct CO 2 electrolysis is suggested to be one of the most economically viable products. However, its commercial viability remains challenging in highly active and selective electrocatalysts. Here, we report that palladium (Pd) doping has a profound positive impact on the electrocatalytic activity of bismuth oxide (Bi 2 O 3 ). The introduction of Pd increases the current density and Faradaic efficiency of HCOOH (FE HCOOH ) in flow cell system. As a result, the optimized Pd-Bi catalyst exhibits a FE HCOOH of 99.1 % at −0.7 (V vs RHE). Operating experimental studies coupled with theoretical calculations reveal that the Pd modified active sites exhibit near-optimal binding energy for the key *OCHO intermediate, which is more conducive to the generation of formic acid. Furthermore, the use of an asymmetric low-frequency pulsed strategy stabilizes the active sites, ensuring sustained catalytic performance. This study highlights the potential of Pd-doped Bi 2 O 3 as a promising candidate for efficient and selective CO 2 electroreduction to formic acid.
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Catalysis Science & Technology
·
2025
·
IF 4.2
Sizhuo Chen,Haoyu Wang,Zhuoyang Fang,Shuang Song,Jie Gao,Weiting Yu
The electrochemical reduction of CO2 (CO2RR) to CO is a highly promising strategy for addressing both environmental and energy challenges. Identifying catalysts with excellent catalytic performance in CO2RR and facile preparation procedures is currently a hot research topic. Herein, a unique series of halogen‐containing polymorphic AgX (X = Cl, Br, I) nanocatalysts with high CO selectivity, activity, and stability in CO2RR have been synthesized via a one-step wet chemical co-precipitation method. A combination of DFT calculations and electrochemical measurements has illustrated that halogen element doping turns the d-band center of Ag shifting closer to the Fermi level, facilitates the interaction between the *COOH intermediate and the catalyst, lowers Gibbs free energy difference (ΔG) for the rate-determining step, and achieves enhanced CO2RR efficiency (CO faradaic efficiency at 93.24%). This study highlighted halogen doping as a strategy for designing efficient and stable electrocatalysts.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Guangming Wang,Junnan Chen,Ye Qu,Yingjun Dong,Keting Wang,Lihua Qian,Rong Fu,Ying Zhang,Hui-Ming Cheng,Xiaolong Zhang
Electrochemical CO 2 reduction (ECR) to produce chemicals and fuel is a promising technique to build a net-zero carbon circular economy. The performance of ECR has largely advanced in the past decade along with the application of gas diffusion electrodes (GDEs). However, the gas-liquid balance in GDEs is highly fragile due to inefficient CO 2 mass transfer in catalyst layers, which is prone to cause the decay of catalytic performance. In this study, integrated Cu electrodes with controllable mesopores are designed and prepared by copolymer mediated electroless deposition. The optimized Cu electrode shows a selectivity of 81 % (including 65 % for C 2 H 4 ) towards C 2+ products, with a maximum C 2+ partial current density of 232 mA∙cm −2 . Further characterization and simulations reveal that the interconnected mesoporous channels stacked by in-situ reduced Cu nanoparticles leads to an improved CO 2 supply near catalytic sites. In addition, a micro-environment boosting the retention, protonation of *CO intermediates and a unique *CO-CHO coupling step is formed. Our findings provide valuable guidance for enhancing mass transfer and C-C coupling in ECR by creating and controlling intrinsic mesoporous structures in catalyst layers.
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ACS Nano
·
2022
·
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 MEMBRANE SCIENCE
·
2024
·
IF 8.4
Yunchuan Pu,Guangwei He,Mingang Zhao,Ziqi Yang,He Li,Yanxiong Ren,Mengying Long,Xuerui Wang,Dan Zhao,Zhongyi Jiang
Two-dimensional metal-organic frameworks (2DMOFs) have emerged as highly appealing candidates as advanced separation membrane materials. However, constructing 2DMOF membranes with appropriate channel sizes to separate CO 2 from N 2 remains a great challenge. Here, we propose an in-situ crystallization approach to synthesize CO 2 -philic-polymer functionalized Zr-based MOF nanosheets, enabling the fabrication of efficient CO 2 capture membranes. The in-situ MOF crystallization with polyethylenimine (PEI) polymers leads to a uniform distribution of amines, resulting in the formation of PEI-NUS hybrid nanosheet characterized by both high porosity and strong affinity to CO 2 . These nanosheets are assembled into ultrathin lamellar membranes with thicknesses ranging from 40 to 120 nm. The amines of PEI polymers significantly facilitate the CO 2 transfer as reaction carriers, resulting in a substantially improved CO 2 /N 2 separation performance with a CO 2 permeance of 410 GPU and a CO 2 /N 2 selectivity of 90, which are among the best for MOF membranes in CO 2 separation. This in-situ functionalization strategy paves the way for the fabrication of ultrathin 2D membranes for various separations.
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Biomass Conversion and Biorefinery
·
2025
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IF 4.1
Zhao Xiaoben,He Tao,Wang Shuainan,He Song
In this research, nitrogen-doped activated carbons (NACs) featuring a high specific surface area (3396 m 2 /g) and a certain amount of nitrogen doping (0.79–1.69%) were prepared by a combination of chemical activation and self-activation methods, and their CO 2 adsorption characteristics were comprehensively assessed. The experimental results showed that nitrogen doping not only significantly enhanced the specific surface area of the materials, but also significantly enhanced the CO 2 adsorption. The CO 2 adsorption capacity of the optimal sample, CMAC-0.5–3-700, reached 4.11 mmol/g and 2.32 mmol/g at 0 °C and 25 °C, respectively. In addition, the selectivity of NACs for CO 2 /N 2 was significantly improved, with a selectivity factor of up to 50.16, and the competitive adsorption experiments also demonstrated that NACs could still effectively adsorb CO 2 under the condition of CO 2 /N 2 = 15/85. Density-functional theory (DFT) calculations further revealed the interaction mechanism between NACs and CO 2 molecules, the enhanced CO 2 selectivity is attributed to electrostatic and π-electron interactions between nitrogen atoms and CO 2 . The findings indicate the significant potential of nitrogen-doped activated carbons (NACs) with high specific surface area and substantial nitrogen doping for post-combustion CO 2 capture.
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Journal of Environmental Chemical Engineering
·
2024
·
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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JOURNAL OF CHEMICAL AND ENGINEERING DATA
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2024
·
IF 2
Xiaodong Shen,Yinde Zhang,Yanxia Li,Long Shen,Jialin Shi,Yang Li
Phase equilibria of carbon dioxide (CO2) hydrate in aqueous solutions of N-methyldiethanolamine (MDEA) at four different mass fractions (5, 10, 15, and 25 wt %) in the temperature range of 274.01 to 281.93 K and pressure range of 1.79 to 4.34 MPa were experimentally investigated by adopting an isochoric pressure search method. The reliability and accuracy of our experimental apparatus and method were examined by comparing the measured data with published ones. The enthalpy of CO2 hydrate dissociation was calculated by the Clausius–Clapeyron equation. The experimental results showed that MDEA acted as a thermodynamic inhibitor which could suppress the equilibrium line of CO2 hydrate to lower temperatures or higher pressures. The thermodynamic inhibition effect was enhanced after increasing the mass fraction. However, it was weaker than the conventional thermodynamic inhibitors of ethylene glycol (EG) and sodium chloride (NaCl). MDEA had synergistic inhibition effects with EG and NaCl, as their mixtures had stronger thermodynamic inhibition performance. The average enthalpies of CO2 hydrate dissociation in the presence of MDEA (5 to 25 wt %) were found to be in the range of 67.562 to 80.776 kJ·mol–1, which were very close to that of pure water. The research results have theoretical guidance for the flow assurance of natural gases.
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Polymers
·
2024
·Vol. 16
·期 3
·393
·
IF 4.7
Xiaoyu Du,Shijun Zhao,Yanqing Qu,Hongge Jia,Shuangping Xu,Mingyu Zhang,Guoliang Geng
Imidazole ionic liquids (ILs) have good affinity and good solubility for carbon dioxide (CO2). Such ionic liquids, combined with polyimide membrane materials, can solve the problem that, today, CO2is difficult to separate and recover. In this study, the ionic liquid (IL) of 1-ethyl-3-methylimidazolium tetrafluoroborate (IL1), 1-pentyl-3-methylimidazolium tetrafluoroborate (IL2), 1-octyl-3-methylimidazolium tetrafluoroborate (IL3), and 1-dodecylimidazolium tetrafluoroborate (IL4) with different contents were added to a polyimide matrix, and a series of polyimide membranes blended with ionic liquid were prepared using a high-speed mixer. The mechanical properties and gas separation permeability of the membranes were investigated. Among them, the selectivity of the PI/IL3membrane for CO2/CH4was 180.55, which was 2.5 times higher than the PI membrane, and its CO2permeability was 16.25 Barrer, which exceeded the Robeson curve in 2008; the separation performance of the membrane was the best in this work.
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PubMed
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ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Pengxuan Wang,Yuming Gao,Haoyu Yan,Zhengwu Yang,Chaoping Xu,Dawei Tang,Bo Jiang
CO 2 methanation offers a practical solution for sustainable, renewable energy storage and long-term space exploration missions. However, conventional direct solar-driven photothermal systems suffer from thermal response hysteresis and dynamic temperature fluctuations, undermining methane yield stability and limiting their applicability under high gas hourly space velocity (GHSV) conditions. Herein, a round-the-clock CO 2 methanation system is pioneered that integrates photovoltaic power generation with induction heating by a rapid-response electromagnetic metamaterial (EEM), serving as both a catalyst and a susceptor. The EMM assembles single atoms, nanoclusters, and nanotubes into a macrostructure by a 3D-printed strategy and rapidly reaches the methanation temperature of 300 °C within just 36 s at a frequency of 297 kHz with an input power of 461 W, achieving a substantially great CH 4 space-time-yield of 821 mmol g cat −1 h −1 at an ultra-high GHSV of 150 000 mL g cat −1 h −1 . The outdoor photovoltaic-driven induction heating system maintains stable production with a cumulative CH 4 output of 1373.2 L over one week, shielding the system from environmental instability. Notably, this system exhibits a solar-to-chemical energy efficiency of 13% and achieves 20% energy savings compared with conventional electric heating technologies, offering a prospective avenue for efficient and stable CO 2 methanation.
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Nano Energy
·
2019
·
IF 15.548
Xiaoli Jin,Chade Lv,Xin Zhou,Haiquan Xie,Shanfu Sun,Yue Liu,Qingqiang Meng,Gang Chen
The insufficient separation of photogenerated charge carriers and faint CO 2 capture remains the major obstacles for photocatalytic conversion of CO 2 into solar fuel. Rational design of semiconductor photocatalysts with unique structures may be promising to break this bottleneck. Herein, bismuth rich Bi 4 O 5 B 2 hollow microspheres are designed as a robust photocatalyst for efficient CO 2 reduction. Thanks to the bismuth rich strategy, the highly dispersed band structure and the elevated conduction band (CB) potential facilitate the charge transfer and photoreduction ability. Meanwhile, hollow structure provides the large specific area and creates a resonance in its interior to enhance the CO 2 adsorption and activation. Benefiting from the collaborative promotion effect, the local charge arrangement and electronic structure are tuned so as to an exceptional efficiency of photocatalytic CO 2 conversion into CO (3.16 μmol g −1 h −1 ) and CH 4 (0.5 μmol g −1 h −1 ) is attained over hollow Bi 4 O 5 Br 2 , which is superior to that of solid Bi 4 O 5 Br 2 and BiOBr, as well as other reported Bi-based photocatalysts. This work paves new opportunities for exploring high-efficiency CO 2 photoreduction catalysts.
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Journal of Energy Chemistry
·
2020
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IF 7.216
Jin-Feng Liao,Ya-Ting Cai,Jun-Yan Li,Yong Jiang,Xu-Dong Wang,Hong-Yan Chen,Dai-Bin Kuang
The optoelectronic performance of CsPbBr 3 nanocrystal (NC) has been dramatically limited by the severe charge carrier recombination and its narrow light absorption range, which are anticipated to be resolved via coupling with plasmonic Au nanoparticle (NP). In view of this, CsPbBr 3 –Au nanocomposite is fabricated and further employed as a concept model to study the electronic interaction between perovskite NC and Au NP for the first time. It has been found that the excitation-wavelength dependent carrier transfer behavior exists in CsPbBr 3 –Au nanocomposite. Upon illumination with visible light ( λ >420 nm), photo-generated electrons in CsPbBr 3 can inject into Au with an electron injection rate and efficiency of 2.84 × 10 9 s −1 and 78%, respectively. The boosted charge separation is further translated into a 3.2-fold enhancement in CO 2 photocatalytic reduction activity compared with pristine CsPbBr 3 . On the other hand, when solely exciting Au NP with longer wavelength light ( λ >580 nm), the localized surface plasmon resonance (LSPR) induced hot electrons in Au NPs can transfer to CsPbBr 3 NC and further participate in photocatalytic reaction towards CO 2 reduction. The present study provides new insights into preparing plasmonic nanostructure to enhance the performance of perovskite based optoelectronic devices.
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