JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Zeyu Wang,Yaling Jia,Shangqing Zhao,Huiling Zheng,Antony Rajendran,Wen-Ying Li
SnO 2 -based materials are promising electrocatalysts for the conversion of CO 2 to formate however increasing their activity further is challenging due to the suboptimal CO 2 adsorption and activation capacity. The interfacial engineering has proven effective in modulating the electronic structure and adsorption behavior of electrocatalysts. Herein, a heterostructure Bi/SnO 2 was constructed for the CO 2 electroreduction to formate in which a formate Faraday efficiency of 94.9 % and single-pass carbon efficiency of 40.3 % were achieved at −1.0 V versus reversible hydrogen electrode in 1.0 M KOH. During a 30-hour stability test, the current density was nearly constant without a significant decrease while the formate Faraday efficiency was maintained around 90 %. This remarkable activity is attributed to the strong electronic interaction arising from p–p orbital coupling at the Bi/SnO 2 interface, according to the experimental and theoretical investigations. The computational insights suggest that the p–p orbital coupling promotes the electron transfer from Bi to SnO 2 and optimizes the adsorption strength of the intermediate (*OCHO) to enhance the catalytic activity. The formation of *OCHO during formate generation was confirmed by the i n situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy. This work might contribute key insights into the mechanisms underlying activity enhancement via strong electronic interaction between dual p- block metal catalysts.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Wenkang Niv,Xu Sun,Xiaoyan Zhang,Zizhong Zhang,Ke Wang,Wenxin Dai,Xianzhi Fu Resource
Photocatalytic CO 2 reduction offers a promising solution to both the energy crisis and environmental issues. However, existing photocatalysts for simulating photosynthesis at ambient temperature exhibit limited conversion efficiency. In this study, we leveraged the photothermal effect of MnO 2 to significantly increase the surface temperature of the catalyst under full-spectrum irradiation, thereby markedly enhancing CO 2 conversion efficiency. Photocatalytic performance evaluations and characterization results revealed that the temperature elevation accelerated the generation and transfer of photogenerated electrons. Furthermore, Cd single atoms (Cd SAs) were successfully incorporated onto the MnO 2 surface through in-situ redox reaction. Various characterizations and first-principles calculations demonstrated that the incorporation of Cd SAs in Cd-MnO 2 created effective atomic-level site for water adsorption and dissociation, providing abundant *H species for CO 2 reduction. Cd SAs also modulate the local electronic environment, facilitating CO 2 adsorption at adjacent Mn sites and lowering the energy barrier for *COOH formation. Moreover, the spin polarization induced by Cd SAs suppresses photogenerated charge recombination while promoting cyclic regeneration of active Mn sites. Furthermore, the weak adsorption of CO on the catalyst hinders its hydrogenation to CH 4 , achieving exceptional CO selectivity (98 %) with a production rate of 318.2 μmol·g −1 ·h −1 . These advantages enhanced thermally-assisted photocatalytic performance, providing valuable insights for improving the efficiency of photocatalytic CO 2 reduction.
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Journal of Materials Chemistry A
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2024
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IF 10.7
Zhihao Zhou,Siyuan Duan,Guangze Nie,Zhenkun Sun,Lunbo Duan
Reverse water-gas shift (RWGS) reaction offers a promising pathway for utilising green H2 to reduce CO2 into CO, a valuable precursor for e-fuel production. Conventional catalyst synthesis methods, however, often rely on costly and complex procedures using fine chemical precursors. In this study, we repurpose retired ternary lithium-ion battery cathodes (rTLIBCs), prevalent e-waste from the electric vehicle industry, as catalysts for the RWGS reaction. Using a straightforward method of mixing rTLIBC material with Al2O3 powder, we successfully synthesise xNCM/Al2O3 catalysts with high CO2 conversion and CO selectivity. Notably, the 10NCM/Al2O3 catalyst demonstrates the highest CO space-time yield at 450–600 °C, with stable performance across long-term tests, maintaining CO2 conversion, CO selectivity, and CO space-time yield. The performance of our prepared catalyst is comparable to that of the best catalysts synthesised using fine chemicals. The high catalytic performance is attributed to the synergistic effect of a Ni-Co bimetallic alloy formed during pretreatment, strong metal-support interaction, and alkali metal Li. Ni-Co alloy formation optimises the catalytic activity and selectivity, the metal-support interaction enhances CO2 activation, and Li boosts basicity and fine-tunes the reaction pathway. This study validates that rTLIBCs are a viable raw material for practical RWGS catalyst synthesis, providing a sustainable alternative for e-waste utilisation.
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ACS Omega
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2025
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IF 4.3
Shuaishuai Zhao,Li Liu,Zhihao Li,Xuliang Fan,Zhiqiang Wang,Mengyi Xing,Fushan Li
CO2 flooding is one of the paramount approaches to ameliorating the oil recovery rate of low-permeability reservoirs. Additionally, the physical and geological characteristics of low-permeability reservoir crude oil are less desirable owing to the influence of continental sedimentary structures. The minimum miscibility pressure (MMP) between CO2 and crude oil is generally higher than the formation fracture pressure, thereby rendering it difficult for CO2 to form miscibility with crude oil. Under such circumstances, a miscibility-reducing agent can be adopted to lower the miscibility pressure between CO2 and crude oil, thus achieving CO2 oil miscible phase flooding and elevating recovery efficiency. This paper first selected the most effective miscibility-reducing agent through molecular simulation experiments and core displacement experiments, and subsequently evaluated the injection effect of the miscibility-reducing agent on heightening the recovery rate of CO2 flooding in low-permeability reservoir cores. This research obtained the effect of the miscibility-reducing agents on the aggregation degree of CO2 molecules and asphaltene molecules during the oil gas mixing process from the radial distribution function and analyzed its function mechanism. On this basis, the core flooding experiment method was adopted to screen for the optimal miscibility-reducing agent with the best miscibility-reducing agent effect. Afterward, the impact of miscibility-reducing agent injection on the CO2 flooding development effect of the low-permeability core was evaluated systematically. As demonstrated by the molecular simulation results, selected miscibility-reducing agents displayed desirable electron transfer ability with CO2; Triisobutyl citrate can effectively heighten the aggregation degree of CO2 molecules and lessen the aggregation degree of asphaltene molecules, with the most conspicuous effect; The results of the core flooding experiment revealed that upon the injection of triisobutyl citrate, the MMP reduction between CO2 and crude oil exhibited the most remarkable trend, so it was selected as the best miscibility-reducing agent. The mechanism by which triisobutyl citrate can effectively reduce MMP mainly includes lowering crude oil viscosity and oil gas interfacial tension, and promoting the CO2 extraction ability. The indoor three-dimensional well network model CO2 flooding experiment results suggested that after injecting 0.07 PV of triisobutyl citrate preflush slug, the CO2 flooding recovery rate increased from 47.78% OOIP without the injection of miscibility-reducing agents to 59.86% OOIP. The selected triisobutyl citrate displayed a striking effect on augmenting the CO2 flooding recovery rate of low-permeability reservoirs. The research results provide a reference and inspiration for the high-quality and efficient development of CO2 flooding in low-permeability oil reservoirs.
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CHINESE JOURNAL OF CATALYSIS
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2024
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IF 15.7
Jiafa Chen,Peng Bai,Shibo Yuan,Yi He,Zifan Niu,Yicheng Zhao,Yongdan Li
Designing highly efficient photocatalyst for the valorization of CO 2 is an ideal strategy to reduce greenhouse gas emissions and utilize solar energy. In this study, a S-scheme heterojunction photocatalyst is fabricated by solvothermal impregnation of ZnO on W 18 O 49 for photocatalytic CO 2 N -formylation of aniline. The localized surface plasmon resonance effect of W 18 O 49 improves the absorption capacity for long-wave light significantly, and the hot electrons generated in W 18 O 49 with a high energy can migrate to the conduction band of ZnO and thus enhance the photocatalytic reduction ability. Meanwhile, the S-scheme heterojunction facilitates the separation of photoinduced charge carriers and preserves the redox ability of W 18 O 49 /ZnO composite photocatalyst. The conversion of aniline reaches 99.1% after 5 h reaction under visible light irradiation at room temperature with an N -formylaniline selectivity of 100%. A possible photocatalytic reaction mechanism is proposed. This study paves a promising way for the design of highly efficient photocatalyst and the sustainable utilization of CO 2 .
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Journal of Materials Chemistry A
·
2025
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IF 9.5
Yi Chen,Weilin Shi,Claudia Li,Kang Hui Lim,Xueqian Wang,Langlang Wang,Ping Ning,Yixing Ma,Sibudjing Kawi
Global warming, driven by rising levels of CO2 in the atmosphere, is an environmental predicament confronted by humanity. Plasma catalytic decomposition of carbon dioxide into carbon monoxide is a practical approach to mitigate this challenge, which can be a crucial step in carbon recycling. Metal selenides are promising candidates owing to their abundant reserves and outstanding electron transfer properties, making them highly active in chemical reactions. In this study, the morphology of AlO(OH) and the dispersion of Cu2−xSe were optimized by hydrothermal synthesis temperature. Specifically, the Cu2−xSe-Al-180 catalyst, prepared at a hydrothermal temperature of 180 °C, formed AlO(OH) with good crystallinity and a nanoscale thin-sheet structure, with Cu2−xSe uniformly distributed on the AlO(OH) support. The reaction of CO2 decomposition to CO production by integrating Cu2−xSe-Al-180 with dielectric barrier discharge (DBD) plasma led to a CO2 conversion of up to 28.07% at a specific input energy (SIE) of 58.07 kJ L−1. The excellent CO2 adsorption properties of AlO(OH) and Cu2Se reduce the activation energy barrier of the reaction, and Cu2Se further promotes the excited activation of CO2 in the plasma. These findings offer valuable insights for the development and design of catalysts in the field of plasma catalysis and highlight the potential of CuSe-based materials in CO2 reduction technologies.
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DALTON TRANSACTIONS
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2025
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IF 3.3
Chaonan Wang,Kaixuan Guo,Zhonghan Cheng,Chongli Wang,Duozhen Chai,Dongfeng Cao,Ye Yuan,Somboon Chaemchuen
Metal-organic frameworks (MOFs) with ZIF-67 have been widely studied. Incorporating multi-bimetals into ZIF-67 offers a strategic approach to leverage unique properties and address the limitations of traditional single-metal in ZIF-67. An environmentally friendly solid-state thermal (SST) method to simultaneously incorporate heterometals (Cu, Fe, Ru, Pd, Mn, and Ni) into the ZIF structure, referred to as M@ZIF-67, is developed. The synthesis occurs in a single step, utilizing thermally-treated mixed solid precursors of multi-bimetals and imidazole ligands without additional agents or solvents, which is the innovative green route to approach multi-bimetals ZIFs. Multiple techniques confirm that heterometals are homogeneous, uniform, and precised metal content in the iso-structure of ZIF-67. Interestingly, synthesizing M@ZIF-67 through the SST method achieves a scalable and high yield. Furthermore, the M@ZIF-67 exhibits a precise heterometal content, which plays a crucial role in enhancing the catalytic performance of CO2 cycloaddition, surpassing results obtained through traditional ZIF-67.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Lei Yuan,Leihao Zhang,Jianpeng Feng,Chongyang Jiang,Jiaqi Feng,Chunshan Li,Shaojuan Zeng,Xiangping Zhang
Electric-driven CO 2 reduction to high value-added chemicals is a potential way to solve the carbon emissions. However, the current studies on CO 2 electroreduction (CO 2 ER) are mainly focused on design and preparation of novel electrocatalysts and electrolytes. The large-scale of CO 2 ER is puzzled in the serious hydrogen evolution reaction (HER) in aqueous electrolytes and inferior reaction stability in an enlarged CO 2 electrolyzer. Ionic liquids (ILs) as electrolytes have opened great opportunities for CO 2 ER due to their unique advantages. Herein, a large-scale CO 2 ER device containing an upscaling modified H-type flow cell using IL-based electrolytes (UHFC-IL) with the largest electrode active area of 495 cm 2 was established for CO 2 ER studies. The influences of key operating parameters, such as compositions of IL-based electrolytes, electrolytes velocity, CO 2 gas flow rate and cell voltage on CO 2 ER performance were systematically investigated. A high CO 2 ER performance under the optimum operating conditions achieves 83.9% Faraday Efficiency (FE) for CO with a reaction current of 6.32 A, suppressing HER to only 2% FE. After 10 hr continuous operation, the CO selectivity in IL-based electrolytes is 51.3% higher than that in 0.1 M KHCO 3 aqueous electrolytes, which maintains excellent stability with a high CO generation rate of 1.7 L hr -1 . In addition, the mechanism of CO 2 ER to CO boosted by IL-based electrolytes in UHFC-IL was proposed. This study provides experimental parameters and guidance for future research on the amplification process of CO 2 ER.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-12
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IF 15.7
Liu Yunlong,Zhang Siyu,Qian Haoyu,Shen Chengbo,Hu Shuijin,Zhang Weijian,Wang Yong,Huang Shan,Wang Songhan,Liu Zhenghui,Li Ganghua,Fu Xiangdong,Ding Yanfeng,Li Shan,van Groenigen Kees Jan,Jiang Yu
Rising atmospheric CO 2 generally increases yield of indica rice, one of the two main Asian cultivated rice subspecies, more strongly than japonica rice, the other main subspecies. The molecular mechanisms driving this difference remain unclear, limiting the potential of future rice yield increases through breeding efforts. Here, we show that between-species variation in the DNR1 ( DULL NITROGEN RESPONSE1 ) allele, a regulator of nitrate-use efficiency in rice plants, explains the divergent response to elevated atmospheric CO 2 (eCO 2 ) conditions. eCO 2 increased rice yield by 22.8–32.3% in plants carrying or mimicking the indica DNR1 allele, but only by 3.6–11.1% in plants carrying the japonica DNR1 allele. Rice plants carrying or mimicking the indica DNR1 allele exhibit decreased eCO 2 -responsive transcription and protein abundance of DNR1, which activates genes involved in nitrate transport and assimilation, driving the increase in plant growth. Our findings identify the indica DNR1 gene as a key breeding resource for sustainably enhancing nitrate uptake and rice yields in japonica varieties, potentially contributing to global food security as atmospheric CO 2 levels continue to increase.
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Small
·
2025
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IF 12.1
Teng Zhang,Xueya Dai,Yihong Yu,Xin Cui,Yunlong Li,Gaowu Qin,Wei Qi,Song Li
Electrochemical conversion of CO 2 into value-added multi-carbon products is highly attractive for CO 2 utilization using sustainable electricity energy. However, achieving high ethanol selectivity of copper-based catalysts remains challenging due to the competing side reactions such as ethylene formation. Herein, a novel electrocatalyst, PANI-Ag/Cu-OH is reported, comprising of polyaniline-supported silver single atoms coupled with hydroxyl-modified copper clusters. Tandem reduction of CO 2 into ethanol with a high selectivity is realized by coupling CO formation on Ag site and further reduction on hydroxylated Cu sites. The synergistic approach enables a high Faradaic efficiency of 68.9% for ethanol with a current density of −263.8 mA cm −2 at −0.78 V versus RHE in alkaline media. CO-TPD and in situ infrared spectra studies reveal that strong CO adsorption and Cu + species stabilized by hydroxyl groups are crucial for asymmetric C–C coupling and stabilization of the ethanol intermediates, leading to the enhanced ethanol selectivity.
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JOURNAL OF MEMBRANE SCIENCE
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2025
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IF 9
Shuangqi Song,Hong Li,Jingde Li,Yanqin Yang
Mixed-matrix membranes (MMMs), developed through the combination of solid fillers with polymer matrices, represent an effective approach addressing the persistent challenge of balancing permeability and selectivity in polymer membrane. Diethylenetriamine-functionalized porous material of PP-DETA, which is synthesized from porous organic polymer of PP via one-step diethylenetriamine grafting, is an ideal material for MMMs production. However, designing and optimizing PP-DETA for high-performance CO 2 separation membranes remains a challenge. Herein, we develop an improved PP-DETA material, designated as PP-DETA-cPIM-1, by covalently attaching a carboxylated polymer of intrinsic microporosity (cPIM-1) network layer onto the PP-DETA surface. Membranes prepared from this PP-DETA-cPIM-1 filler and PIM-1 matrix demonstrate enhanced interfacial adhesion and stronger mechanical properties in comparison to the counterparts with the same loading of PP-DETA. The incorporation of PP-DETA-cPIM-1 into MMMs establishes an enhanced filler/polymer interface that facilitates the selective transport of CO 2 through the filler, while simultaneously improving membrane stability and suppressing physical aging. Specifically, with 5 wt% loading of PP-DETA-cPIM-1 filler, the MMM is able to enhance the CO 2 /N 2 selectivity and CO 2 permeability by 52.3 % and 25.3 %, respectively, exceeding the upper bound established in 2008. Furthermore, PP-DETA-cPIM-1/PIM-1 MMMs display superior anti-aging ability for 180 days of aging.
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INORGANIC CHEMISTRY
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2025
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IF 4.7
Shunsheng Ye,Feng Wang,Liying Zhang,Fuqiang Fan,Xuemin Zhang,Tieqiang Wang,Yu Fu
The catalytic performance of 2D nanostructure-based heterogeneous catalysts is highly dependent on their dispersibility and stability. This work presents the grafting of polymer brushes onto 2D Cu-based metal–organic framework (MOF) nanoplates via a versatile UV-induced radical polymerization approach for CO2 fixation through the cycloaddition reaction with epoxides. The polymer brushes are selectively anchored to the external surfaces of the nanoplates, which greatly improves the long-term dispersibility and stability in solvents while preserving their intrinsic porosity and crystalline structures. The poly(N,N-dimethylaminoethyl methacrylate)-grafted 2-aminoterephthalic acid copper (CuBDC-NH2@PDMAEMA) nanoplates, with an optimized polymer brush thickness, achieve a maximum yield of 81.2% in the cycloaddition of CO2 with styrene oxide, which is a 1.6-fold improvement over that of the unmodified CuBDC-NH2 nanoplates. The grafted nanoplates also exhibit excellent recyclability with a slight decrease in yield after multiple consecutive cycles. The versatility of this approach is further demonstrated by its application to other polymers and epoxide substrates, where polymer-grafted catalysts consistently outperform their pristine counterparts. Our strategy provides a feasible and efficient route to synthesize MOF/polymer hybrid nanomaterials for sustainable CO2 utilization and green chemistry applications.
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