Materials
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2025
·Vol. 18
·期 14
·3419
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IF 3.2
Muhammad Sabir,Mahmoud Sayed,Iram Riaz,Guogen Qiu,Muhammad Tahir,Khuloud A. Alibrahim,Wang Wang
The rapid recombination of photoinduced charge carriers in semiconductors remains a significant challenge for their practical application in photocatalysis. This study presents the design of a step-scheme (S-scheme) heterojunction composed of carbon nitride (g-C3N4) and nickel-based metal–organic framework (Ni-MOF) to achieve enhanced charge separation. The establishment of an S-scheme charge transfer configuration at the interface of the Ni-MOF/g-C3N4heterostructure plays a pivotal role in enabling efficient charge carrier separation, and hence, high CO2photoreduction efficiency with a CO evolution rate of 1014.6 µmol g−1h−1and selectivity of 95% under simulated solar illumination. CO evolution represents an approximately 3.7-fold enhancement compared to pristine Ni-MOF. Density functional theory (DFT) calculations, supported by in situ irradiated X-ray photoelectron spectroscopy (XPS) and electron paramagnetic resonance (EPR) experimental results, confirmed the establishment of a well-defined and strongly bonded interface, which improves the charge transfer and separation following the S-scheme mechanism. This study sheds light on MOF-based S-scheme heterojunctions as fruitful and selective alternatives for practical CO2photoreduction.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Xingwang Zhu,Xiang Liu,Xiang Shi,Fujiang Huang,Hangmin Xu,Ganghua Zhou,Xiaozhi Wang,Xu Dong,Penghui Ding,Jianning Ding,Hui Xu
The surface of photocatalysts plays a key role in the adsorption and activation of CO 2 molecules. Establishing the conformational relationship between the crystalline phase of the photocatalysts and the CO 2 reduction reaction (CO 2 RR) activity is crucial to understanding the catalytic reaction mechanism. Herein, we synthesized CdS catalysts with different exposed crystalline facets (CdS[100], CdS[001], and CdS[111]) using hydrothermal and water bath methods and evaluated their photocatalytic CO 2 RR performances. The results showed that CdS[001] displayed an optimal activity with a 203.2 μmol g −1 h −1 of CO generation rate compared with CdS[100] and CdS[111]. More importantly, the CdS[001] catalyst shows the best CO selectivity ( S CO : ~ 86.6 %) and CO 2 reduction selectivity ( S CO2 : ~95.4 %) compared with CdS[100] ( S CO : 79.3 %; S CO2 : 90.0 %) and CdS[111] ( S CO : 79.6 %; S CO2 : 82.8 %). The optimal CdS[001] catalyst significantly inhibited the competing hydrogen evolution reaction. The adsorption and activation behaviors of CO 2 on various exposed surfaces of CdS are explored in depth based on density functional theory calculations and in-situ Fourier transform infrared spectra measurements. This work provides new insights into understanding the role of facet control in enhancing photocatalytic CO 2 conversion.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Liangwei Hu,Yi Zhang,Junzhu Yang,Qi Xia,Huipeng Gao,Lanpeng Li,Hongxin Zhao,Jin Zhang,Quan Zhang,Yuan Lu
Currently, electrocatalytic conversion of carbon dioxide into higher-value compounds is a promising approach. However, developing a stable and efficient catalyst with high selectivity for specific products remains a major challenge. Herein, we constructed a bismuth-based metal-organic framework (Bi-MOF) as a catalyst for the catalytic production of formic acid from carbon dioxide, to which different ratios of tin metal elements were doped. The catalyst Bi-MOF Sn6 exhibited excellent catalytic performance, with a formic acid selectivity of 80 % at −1.8 V and a current density of 25 mA/cm 2 . The catalytic mechanism of electrocatalytic CO 2 reduction reaction (ECO 2 RR) was revealed using density functional theory calculations. The work demonstrated that tin metal doping in Bi-MOF could effectively promote the catalytic process of ECO 2 RR, providing valuable insights for the subsequent design of more commercially available ECO 2 RR catalysts and more efficient CO 2 reduction systems.
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Cell Reports Physical Science
·
2025
·
IF 7.3
Weiqiang Wang,Weifeng Zhang,Fengjiao Chu,Tingting Xiao,Dongdong Hu,Pengyi Tang,Jiajia Gao,Honghua Ge
The release of CO 2 has challenged the worldwide environment and led to climate change. An emerging solution is to construct bio-abiotic semiartificial photocatalysis systems for the highly efficient conversion of CO 2 . However, biocompatibility and the narrow product spectrum are challenging these bio-abiotic photocatalysis systems integrating living cells and semiconductors. Living bacterial biofilms can provide a large specific surface area for photosensitizer mineralization, allowing CO 2 fixation, one-carbon product uptake, and further assimilation. Here, we report a living photosensitizer-mineralized biofilm platform with a biocompatible and stable bio-abiotic interface conducting single-enzyme to whole-cell photocatalytic applications. Such engineered photosensitizer-mineralized biofilms not only efficiently implement the regeneration of NADH but also enable the conversion of CO 2 into formate and finally into polyhydroxyalkanoates under light illumination. Thus, this work demonstrates an alternative approach to solar-to-chemical conversion. The proof of concept established in this work might be used for other sustainable photocatalytic applications.
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ChemCatChem
·
2025
·
IF 3.9
Xiang Xia,Yudong Wu,Xiao Liu,Yajie Liang,Kai Liu
Graphical Two systems including electrolysis-purification system (System I) and direct-electrolysis system (System II) were evaluated for their efficiency to produce fatty acid using cupriavidus sp. XH293. Our results shows that Sytem I was more favorable with higher yield of fatty acid, suggesting that decoupled electrochemical and microbial catalysis can be an efficient approach for CO 2 fixation driven by renewable energy. The heavy reliance on fossil fuels results in excessive greenhouse emissions, exacerbating environmental change, and global warming. CO 2 electrocatalysis has been widely studied and the products are limited to C 1-2 . Herein, we reported the integration of electrocatalysis and microbial catalysis for the synthesis of fatty acids from CO 2 . Here, we compared two decoupled MESs for fatty acid production, electrocatalysis-purification system (System I), and direct-electrocatalysis system (System II). Firstly, an upstream electrolysis was used to reduce CO 2 to formate using KHCO 3 and medium as electrolyte, respectively, with carbon nanofiber supported bismuth (Bi@PCF) catalyst. The results indicated that KHCO 3 as electrolyte had higher formate yield and Faraday efficiency than that of medium. Subsequently, a downstream microbial catalysis composed of Cupriavidus species was employed to synthesize fatty acids from formate in System I and System II, respectively. It was demonstrated that System I with the yield of 1.006 mg L −1 was more favorable for the synthesis of fatty acids than System II with the yield of 0.349 mg L −1 . These results suggested that decoupled electrochemical and microbial catalysis were an efficient approach for fixing CO 2 , indicating the great potential of a renewable energy driving artificial photosynthesis.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2025
·
IF 3.9
Dingyue Zhang,Yan Shao,Huanhao Chen
This study reports the mechanochemical synthesis of a highly efficient multicomponent CuInZnZrOx catalyst for the sorption-enhanced hydrogenation of CO2 to methanol. Through systematic optimization, the catalyst with a suitable indium loading of 0.5 wt % demonstrated favorable catalytic performance, achieving 22.5% CO2 conversion and 77.8% methanol selectivity under optimized reaction conditions (240 °C, 5 MPa, H2/CO2 = 10:1). Comprehensive structural characterization revealed that the incorporation of indium species significantly enhanced the dispersion of Cu nanoparticles while stabilizing the active Cu+/Cu0 sites, which are critical for both CO2 activation and methanol synthesis. The optimized CuIn0.5ZnZrOx catalyst exhibited remarkable long-term stability, maintaining over 95% of its initial activity during a 1000-h durability test, with a peak methanol space-time yield reaching 1974 g kgcat–1 h–1. Furthermore, when integrated with 13X zeolite in a sorption-enhanced reactor system, the catalyst system achieved a dramatic improvement in CO2 conversion (up to 65%), attributed to the in situ removal of the byproduct water that shifted the reaction equilibrium. This work not only elucidates the synergistic effects between indium modification and sorption-enhanced engineering but also presents a scalable and sustainable strategy for efficient CO2-to-methanol conversion, offering significant potential for industrial applications in carbon capture and utilization.
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Journal of Energy Chemistry
·
2025
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IF 14.9
Jiangtao Yang,Yunzhen Jia,Guang Liu,Dazhong Zhong,Jinping Li,Qiang Zhao
The metallic Ni catalyst suffers from strong binding with the *CO intermediate, resulting in poisoning of the catalyst surface. It is feasible to facilitate the generation of CO by alleviating the binding strength of the *CO intermediate on the Ni metal surface through a lattice expansion strategy. Here, Ni 3 ZnC 0.7 @C with lattice expansion was synthesized by co-doping with Zn and interstitial C through high-temperature pyrolysis. Structural characterization confirms that the lattice of Ni 3 ZnC 0.7 expands by 5.47% compared to Ni due to the co-doping of Zn and interstitial C. The Ni 3 ZnC 0.7 @C possesses excellent catalytic performance with Faradaic efficiency (FE) of CO exceeding 90% over a wide potential range from −0.8 to −1.4 V versus reversible hydrogen electrode (vs. RHE) with a peak FE CO of 96.6% at −1.0 V vs. RHE. In membrane electrode assembly (MEA) testing, Ni 3 ZnC 0.7 @C achieves a FE CO of 81.4% at the industrial-level current density of 400 mA cm −2 . In situ attenuated total reflection surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) and density functional theory (DFT) calculations reveal that the co-introduction of Zn and interstitial C in the Ni crystal can significantly promote the desorption of *CO intermediate, which facilitates the generation of CO. This study demonstrates a viable way for designing efficient transition metal catalysts for CO 2 electroreduction through lattice strain engineering.
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ENERGY & FUELS
·
2025
·
IF 5.3
Runfen Zheng,Lixin Wei,Yuxin Bai,Jianfei Man,Jian Ye,Huiping Zhang,Yihan Wang
To address the issues of poor regeneration performance and high regeneration energy consumption associated with traditional CO2 absorbents, the development of novel phase-change absorbents has become a key area of research. In this study, a new phase-change absorbent system, DEGDEE-AEEA-AMP, is developed, using N-(2-hydroxyethyl)ethylenediamine (AEEA) as the main absorbent, bis(2-ethoxyethyl)ether (DEGDEE) as the phase-separation agent, 2-amino-2-methyl-1-propanol (AMP) as the activator, and water as the solvent. The performance of this system is compared with that of monoethanolamine (MEA) at a 30% mass concentration, which serves as the reference standard. The study includes absorption, desorption, corrosion, cyclic absorption–desorption experiments, and regeneration energy consumption estimations. The results indicate that the volume of the rich phase in the DEGDEE-AEEA-AMP (DAP) system constitutes 56.7% of the total volume. When the AMP mass fraction is 15%, the absorption capacity reaches 2.52 mol·kg–1, which is 14.0% higher than that of MEA. The maximum desorption rate is 13.19 × 10–3 mol·kg–1·s–1, which is 3.39 times higher than that of MEA. The minimum regeneration energy consumption is 2.742 GJ·t–1 CO2, representing a 29.9% reduction compared to 30% MEA. The corrosion rate of the rich liquid is 0.230 mm/a, 1.32 times that of MEA, but it can be significantly reduced by adding anhydrous Na2SO3. When the AMP mass fraction is 15%, the DAP phase-change absorbent system exhibits high absorption and desorption performance, good cyclic stability, and lower regeneration energy consumption.
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Nature Communications
·
2025
·Vol. 16
·期 1
·10493
·
IF 15.7
Zhang Zhiyong,Huang Qing,Xie Yangen,Zhang Boyang,Zhao Qi,Huang Xingmiao,Yang Na,Ji Hongwei,Chen Chuncheng,Sheng Hua,Zhao Jincai
Current CO 2 utilization depends on high-purity CO 2 , necessitating energy-intensive capture and purification from air. Herein, we present a practical system that selectively converts atmospheric CO 2 with ammonia into urea using solar energy as the sole input. This system is enabled by a heterostructure composed of an indium–porphyrin metal–organic framework and UiO-66-NH 2 , which harness ambient O 2 to promote rather than suppress CO 2 reduction. As a result, it achieves a CO production rate of 272.1 μmol·g −1 ·h −1 directly from air, which is competitive compared to the systems that rely on high-purity CO 2 . Moreover, coupling atmospheric CO 2 reduction with ammonia oxidation enables direct air-to-urea conversion with high selectivity. A scaled-up prototype operating under natural sunlight and open-air conditions achieves a urea production rate of 32.4 μmol·g −1 ·h −1 . This work integrates atmospheric CO 2 capture, solar-driven conversion, and product collection within a single, scalable platform, offering a practical route for carbon utilization under real-world conditions.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-12
·
IF 15.7
Li Jieyang,Zhang Huanlei,Luo Changhao,Cheng Dongbo,Xu Wanping,Lin Meng
Electrochemical conversion of CO 2 into fuels represents an important pathway for addressing the challenges of climate change and energy storage. However, large-scale applications remain hindered by the instability and inefficiency of CO 2 reduction systems, particularly under highly alkaline electrolytes and high current densities. One primary obstacle is the cathodic salt precipitation, which hinders mass transfer and blocks active sites limiting the lifespan of these systems. Here, we present a non-isothermal strategy that leverages a thermal gradient across the membrane electrode assembly to enhance electrochemical performance and suppress salt precipitation. By maintaining a cooler cathode and warmer anode, we exploit the Soret effect to drive cations away from the cathode, mitigating salting-out while boosting anodic activity and cathodic CO 2 solubility. The non-isothermal case has demonstrated over 200 h of stable operation at 100 mA cm −2 under highly alkaline conditions, outperforming conventional isothermal systems. Techno-economic analysis reveals reductions in CO 2 -to-CO production costs, supporting the scalability of this strategy. These findings enable the practical deployment of stable, high-efficiency CO 2 electrolysis systems.
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ENERGY & FUELS
·
2025
·
IF 5.3
Hao Li,Zhuo Chen,Rongxin Xia,Ze Zhang,Junhu Zhou,Yu-You Li,Jun Cheng
To simultaneously promote both direct (via electron carriers) and indirect electron transfer (via hydrogen carriers) in the microbial electroreduction of CO2 to CH4, FeCoCrNiMo high-entropy alloys (HEAs) combined with methanogens were proposed herein. Experimental results showed that spherical HEA heterostructures significantly enhanced the electrical conductivity and catalytic activity. FeCoCrNiMo HEAs increased the abundance of hydrogenotrophic methanogens (e.g., Methanobacterium) and electroactive bacteria (e.g., Ureibacillus), as well as the expression of conductive pilus-associated gene (pilA) to promote electron transfer. FeCoCrNiMo HEAs also increased the content of aromatic proteins and tryptophan in extracellular polymeric substances, enhancing biofilm conductivity, while the uniform dispersion of the five metal elements reduced both biofilm resistance and charge transfer resistance. Therefore, HEAs enhanced the maximum methane production rate by 6.58 times (2.17 mmol L–1 day–1) with 90.6% faradaic efficiency. This study demonstrated that FeCoCrNiMo HEAs promoted electron shuttling efficiency, biofilm electroactivity, and stability, highlighting their potential as multifunctional promoters for driving CO2 reduction to methane.
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2025
·
IF 14.3
Zhiyuan Liu,Qixuan Xiang,Hao Zhang,Xianglong Zhang,Huijun Tan,Yaping Zhao
Mechanochemical ball milling is a straightforward and efficient technology for material synthesis. However, cold welding significantly hampers both the reaction rate and the powder yield of the ball milling process. This study introduces a novel strategy to mitigate cold welding by utilizing supercritical carbon dioxide (SCCO 2 ) as a process control agent. The mechanism by which SCCO 2 inhibits cold welding was elucidated: SCCO 2 reduces surface energy and passivates dangling bonds on the newly exposed surfaces generated by ball milling, thereby preventing undesired re-formation. Building on this approach, a groundbreaking SCCO 2 -driven ball milling (SDBM) method was developed, enabling the one-step, scalable production of 100 g of binary spinel oxide at room temperature within 8 h. Remarkably, the powder yield increases significantly from 13% (conventional ball milling) to 98%. The synthesized spinel oxide exhibits a small particle size, enhanced Mg migration, abundant oxygen vacancies, and high electrochemical performance (385 C/g for MgCo 2 O 4 ). Beyond MgCo 2 O 4 , various binary and ternary spinel oxides were fabricated using SDBM technology. These results highlight the considerable benefits and the universality of SDBM technology in the fabrication of innovative materials.
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