CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Shuangshuo Li,Yongjing Hao,Xionglei Wang,Zheng Zhu,Fan Li,Jiaojiao Zhao,Tian Tian,Tao Chang
In addressing the critical challenge of achieving functional synergy in sustainable materials, this study introduces an innovative ionic-pair strategy to construct amino acid-derived green organic polymer frameworks with specifically tailored active sites for CO 2 adsorption and conversion, devoid of halide anions and metal ions. The intrinsic properties and microstructure of these polymers were meticulously modulated through ionic-pairing between amino acid monomers. Comprehensive characterizations and molecular dynamic simulations systematically verified the presence of dual-active sites and stability of the architecture. Experimental and kinetic analyses indicate that these polymers exhibit exceptional performance in CO 2 adsorption capacity and catalytic conversion, with an activated energy of 15.76 kcal·mol −1 . Furthermore, the adsorption and catalytic mechanisms were extensively investigated using the Monte Carlo method and density functional theory calculations. The amino group in AMA-Glu effectively adsorbs and activates CO 2 , while epoxides undergo nucleophilic attack by the carboxylate anion, facilitating ring-opening reactions. The synergistic interaction between the two groups promotes the cycloaddition reaction. Under conditions devoid of co-catalyst, solvent, and halogen at 80 °C for 8 h, the yield of cyclic carbonates achieved 94.3 %, demonstrating strong competitive performance. This study offers substantial theoretical and practical insights into the utilization of green organic catalytic materials for CO 2 conversion.
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-12
·
IF 14.7
He Xiaoyang,Lin Li,Li Xiangying,Zhu Minzhi,Zhang Qinghong,Xie Shunji,Mei Bingbao,Sun Fanfei,Jiang Zheng,Cheng Jun,Wang Ye
The membrane electrode assembly (MEA) is promising for practical applications of the electrocatalytic CO 2 reduction reaction (CO 2 RR) to multi-carbon (C 2+ ) compounds. Water management is crucial in the MEA electrolyser without catholyte, but few studies have clarified whether the co-feeding water in cathode can enhance C 2+ formation. Here, we report our discovery of pivotal roles of a suitable nanocomposite electrocatalyst with abundant Cu 2 O−Cu 0 interfaces in accomplishing water-promoting effect on C 2+ formation, achieving a current density of 1.0 A cm −2 and a 19% single-pass C 2+ yield at 80% C 2+ Faradaic efficiency in MEA. The operando characterizations confirm the co-existence of Cu + with Cu 0 during CO 2 RR at ampere-level current densities. Our studies reveal that Cu + works for water activation and aids C‒C coupling by enhancing formations of adsorbed CO and CHO species. This work offers a strategy to boost CO 2 RR to C 2+ compounds in industrial-relevant MEA by combining water management and electrocatalyst design.
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Molecular Catalysis
·
2024
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IF 3.9
Chi Ma,Zhiyong Zhong,Quanjun Xiang
The photocatalytic efficiency of bismuth-based metal-organic framework (Bi-MOF) is extremely restricted by the rapid recombination of photogenerated electron-hole pairs, which reduce the number of electrons involved in the photocatalytic reduction reaction. Constructing precise interfacial bond bridges between metal nanoparticles (NPs) and MOFs has emerged as an effective strategy to address the above-mentioned issues, promoting the electrons transfer. Herein, this study improves the sluggish dynamics of photogenerated charge in Bi-MOF by inducing the Pd-O-Bi bond bridges at the interface on a Pd NPs-decorated Bi-MOF (Pd/Bi-MOF) nanosheets. This phenomenon results in an interaction between Pd NPs and the Bi-MOF support. And Pd-O-Bi bond bridges provide the fast electron transfer channels, triggering the directional migration of photogenerated electrons from Pd to Bi node, then enhancing the spatial separation of photogenerated electron-hole pairs, finally facilitating overall photocatalytic CO 2 reduction. The presence of these bond bridges leads to higher enhancement in CO production for Pd/Bi-MOF nanosheets compared to the Bi-MOF nanosheets under visible light irradiation after 4.5 h. This research demonstrates the importance of interfacial bond bridges and provides a reasonable guide to design efficient photocatalyst for reduction of CO 2 to CO.
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Journal of Materials Chemistry A
·
2024
·Vol. 12
·期 28
·17181-17192
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IF 10.7
Chen Yu,Taoning Lei,Li Xu,Chuyao Jin,Jundong Yi,Shenghui Liu,Saisai Lin,Yang Yang,Hao Song,Kaige Wang,Haidong Fan,Chenghang Zheng,Xiao Zhang,Xiang Gao
Establishing a suitable electrode microenvironment is important to achieving high-efficiency electrocatalytic CO2 reduction at industrially relevant current densities. Introducing ionomers provided an effective method for regulating the electrode microenvironment, but the mechanism of interactions between the ionomer and the catalyst remains elusive. In this work, the influence of three types of ionomers on the performance and microenvironment of Ag nanoparticle (NP) and molecularly dispersed cobalt phthalocyanine (CoPc MDE) catalysts were systematically investigated. It was found that the non-covalent interactions between the ionomers with aromatic groups and CoPc MDE resulted in the hydrophilicity of electrode and undesirably promoted the generation of hydrogen during the reaction. The optimal ionomer–catalyst combinations achieved excellent FE(CO)s > 99% at current densities up to −200 mA cm−2 and stable operation for more than 180 h at a current density of −100 mA cm−2. This work underlines the necessity of selecting appropriate ionomer according to the nature of catalyst.
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FUEL
·
2025
·
IF 7.5
Cuncun Qian,Ming-Jia Li,Ruilong Wang
Solar-powered photocatalytic CO 2 reduction offers great potential for carbon fixation. Conventional wide-bandgap semiconductors absorb little visible light. Dye sensitization improves absorption but reduces photoelectron transfer efficiency, limiting photocatalytic performance. This work reports a self-sensitized anatase brown titanium dioxide (B-TiO 2 ) catalyst developed through an optimized two-step method. Comprehensive experimental and computational analyses reveal that B-TiO 2 extends its spectral absorption edge to 601.94 nm, over 43.69 % compared to P25, significantly enhancing visible light absorbance. The surface of B-TiO 2 characterized by oxygen vacancies, Ti 3+ species, and lattice defects, which are crucial for its markedly improved photocatalytic activity. Under irradiation from a 300 W Xe-lamp, the self-sensitized B-TiO 2 catalyst achieves an impressive total charge-transferred electron number of 570.84 μmol·g −1 ·h −1 and a CO 2 conversion rate of 142.05 μmol·g −1 ·h −1 . Furthermore, the photocatalytic mechanism was investigated in detail. This innovative self-sensitized catalyst offers a promising strategy for developing high-efficiency photocatalysts, potentially advancing the field of photocatalytic CO 2 reduction.
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JOURNAL OF THE ENERGY INSTITUTE
·
2024
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IF 5.6
Zheng Bo,Mengyu Cao,Yaolin Wang,Jianhua Yan,Kefa Cen,Xin Tu
Plasma catalytic CO 2 hydrogenation has emerged as a promising approach for converting CO 2 into valuable chemicals such as CO, offering a potential solution to mitigate greenhouse gas emissions. In this study, we investigate the synergistic effect between plasma and a Cu/Ti 3 C 2 T x MXene catalyst for CO 2 hydrogenation via the reverse water gas shift (RWGS) reaction in a dielectric barrier discharge (DBD) reactor. Our findings reveal a significant enhancement in CO 2 conversion (33.1%) and CO yield (31.9%) when using the Cu/Ti 3 C 2 T x catalyst compared to plasma alone or with a Ti 3 C 2 T x foam. Plasma treatment creates unsaturated Ti sites on the Ti 3 C 2 T x surface, dramatically improving CO 2 adsorption and activation, while Cu nanoparticles significantly enhances the activation and dissociation of H 2 molecules on the catalyst surface. These surface adsorbed hydrogen species readily hydrogenate adsorbed CO 2 molecules through the Langmuir-Hinshelwood mechanism. Furthermore, these surface hydrogen species can also participate in the conversion of gas-phase CO 2 molecules through the Eley-Rideal pathway. This work sheds light on the synergistic plasma catalytic mechanism and provide insights for optimizing CO 2 hydrogenation processes using MXene catalysts.
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Energy Technology
·
2024
·
IF 3.6
Xueli Zhang,Shan Hu,Fangyuan Zhang,Shuchen Xing,Huilin Hu,Jinhua Ye,Defa Wang
As a promising technology to mitigate global carbon emissions, photothermal catalytic CO 2 reduction remains a great challenge in increasing the conversion efficiency and regulating the product selectivity. Herein, a series of phase-separated Ni–Mo alloy catalysts for efficient photothermal CO 2 reduction with tunable CO selectivity is reported. With the increase of Mo content, the evolution rate and selectivity of CO increases. The optimal catalyst Ni 1 Mo 1 achieves 32.1% CO 2 conversion with 98.0% of CO selectivity and 71.1 mmol g cat −1 h −1 of CO evolution rate under a 300 W xenon lamp irradiation. Further increasing the Mo content reduces the CO evolution rate while maintaining the high CO selectivity. In the mechanistic study, it is revealed that the Ni–Mo alloy with an appropriate Ni/Mo ratio (e.g., Ni 1 Mo 1 ) possesses a modified electronic structure with more negative d-band center, which increases the light absorption, reduces the H 2 dissociation, and favors the CO desorption, thereby leading to efficient and selective photothermal reduction of CO 2 to CO. In this work, a viable strategy to design nickel-based catalysts is provided for efficient and selective photothermal CO 2 reduction via composition-mediated modification of electronic structure.
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LANGMUIR
·
2024
·
IF 3.7
Zhuoxue Li,Yunlei Shi,Yimian Ding,Dazhen Xiong,Zhiyong Li,Huiyong Wang,Jikuan Qiu,Xiaopeng Xuan,Jianji Wang
A Pickering emulsion is a natural microreactor for interfacial catalysis in which an emulsifier is critical. Recently, a metal–organic framework (MOF) has attracted attention to emulsify water–organic mixtures for constructing a Pickering emulsion. However, a few stimuli-responsive Pickering emulsions based on MOFs have been reported, and the MOF emulsifiers cannot be regenerated at room temperature. Herein, the Zr-MOF with a rodlike morphology is synthesized using ionic liquid as a modulator and then modified with n-(trimethoxysilylpropyl)imidazole (C3im) to prepare a series of functionalized Zr-MOFs (MOF-C3im). It is found that MOF-C3im is an excellent emulsifier to construct stable and CO2-responsive Pickering emulsions even at low content (>0.20 wt %). Notably, the emulsification and demulsification of the emulsions can be easily and reversibly switched by bubbling of CO2 and N2 alternatively at room temperature because CO2 and imidazole molecules anchored on the Zr-MOF underwent a reversible acid–base reaction, resulting in an obvious change in the wettability of the emulsifier. As a proof of concept, the reduction reactions of nitrobenzene have been successfully carried out in these Pickering emulsions, demonstrating the efficient integration as a microreactor for chemical reaction, product separation, and emulsifier recycling under ambient conditions. This strategy provides an innovative option to develop stimulus-responsive Pickering emulsions for sustainable chemical processes.
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-9
·
IF 14.7
Zhai Jianxin,Xia Zhanghui,Zhou Baowen,Wu Haihong,Xue Teng,Chen Xiao,Jiao Jiapeng,Jia Shuaiqiang,He Mingyuan,Han Buxing
Upcycling of CO 2 into fuels by virtually unlimited solar energy provides an ultimate solution for addressing the substantial challenges of energy crisis and climate change. In this work, we report an efficient nanostructured Ru/MnO x catalyst composed of well-defined Ru/MnO/Mn 3 O 4 for photo-thermal catalytic CO 2 hydrogenation to CH 4 , which is the result of a combination of external heating and irradiation. Remarkably, under relatively mild conditions of 200 °C, a considerable CH 4 production rate of 166.7 mmol g −1 h −1 was achieved with a superior selectivity of 99.5% at CO 2 conversion of 66.8%. The correlative spectroscopic and theoretical investigations suggest that the yield of CH 4 is enhanced by coordinating photon energy with thermal energy to reduce the activation energy of reaction and promote formation of key intermediate COOH* species over the catalyst. This work opens up a new strategy for CO 2 hydrogenation toward CH 4 .
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ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Chengqi Guo,Enhui Jiang,Qiuli Chen,Wanhe Li,Yahui Chen,Shuhan Jia,Yiying Zhou,Zhonghuan Liu,Xinyu Lin,Pengwei Huo,Chunxiang Li,Yun Hau Ng,John Charles Crittenden,Zhi Zhu,Yan Yan
Efficient photocatalytic solar CO2 reduction presents a challenge because visible-to-near-infrared (NIR) low-energy photons account for over 50% of solar energy. Consequently, they are unable to instigate the high-energy reaction necessary for dissociating C═O bonds in CO2. In this study, we present a novel methodology leveraging the often-underutilized photo-to-thermal (PTT) conversion. Our unique two-dimensional (2D) carbon layer-embedded Mo2C (Mo2C–Cx) MXene catalyst in black color showcases superior near-infrared (NIR) light absorption. This enables the efficient utilization of low-energy photons via the PTT conversion mechanism, thereby dramatically enhancing the rate of CO2 photoreduction. Under concentrated sunlight, the optimal Mo2C–C0.5 catalyst achieves CO2 reduction reaction rates of 12000–15000 μmol·g–1·h–1 to CO and 1000–3200 μmol·g–1·h–1 to CH4. Notably, the catalyst delivers solar-to-carbon fuel (STF) conversion efficiencies between 0.0108% to 0.0143% and the STFavg = 0.0123%, the highest recorded values under natural sunlight conditions. This innovative approach accentuates the exploitation of low-frequency, low-energy photons for the enhancement of photocatalytic CO2 reduction.
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Gas Science and Engineering
·
2024
·
IF 0
Xuebi Du,Dawei Shao,Yinhua Wan
Metal-organic frameworks (MOFs) have shown potential as nanofillers for the selective capture of specific gases in mixed matrix membranes (MMMs). This study introduces an efficient method, utilizing a mild (100 °C) reaction condition and a short reaction time (20 min), for the synthesis of MOF-808(Ce) nanocrystals. The MOF-808(Ce) that is obtained exhibits porous characteristics, a notable affinity for CO 2 , and robust intermolecular interactions with PIM-1. Furthermore, this study pioneers the incorporation of MOF-808(Ce) as a filler into PIM-1, with varying loadings, to create PIM/MOF-808 MMMs for the purpose of CO 2 separation. Consequently, the MMMs containing 2 wt% MOF-808(Ce) demonstrate high CO 2 permeability of 6854 Barrer and CO 2 /N 2 selectivity of 23.2, which is far surpasses 2008 upper bound from Robeson and approaches the refined 2019 upper bound from MeKenow. A comparative analysis demonstrates the efficacy of MOF-808(Ce) as a filler in PIM-1 for the purpose of CO 2 separation.
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Journal of Energy Chemistry
·
2024
·
IF 14
Liangping Xiao,Qizheng Zheng,Rusen Zhou,Sifan Liu,Yifan Zhao,Yadong Zhao,Renwu Zhou,Kostya Ken Ostrikov
The electrochemical carbon dioxide reduction (eCO 2 RR) to formate, driven by clean energy, is a promising approach for producing renewable chemicals and high-value fuels. Despite its potential, further development faces challenges due to limitations in electrocatalytic activity and durability, especially for non-noble metal-based catalysts. Here, naturally abundant bismuth-based nanosheets that can effectively drive CO 2 -to-formate electrocatalytic reduction are prepared using the plasma-activated Bi 2 Se 3 followed by a reduction process. Thus-obtained plasma-activated Bi nanosheets (P-BiNS) feature ultrathin structures and high surface areas. Such nanostructures ensure the P-BiNS with outstanding eCO 2 RR catalytic performance, highlighted by the current density of over 80 mA cm −2 and a formate Faradic efficiency of >90%. Furthermore, P-BiNS catalysts demonstrate excellent durability and stability without deactivation following over 50 h of operation. The selectivity for formate production is also studied by density functional theory (DFT) calculations, validating the importance and efficacy of the stabilization of intermediates (*OCHO) on the P-BiNS surfaces. This study provides a facile plasma-assisted approach for developing high-performance and low-cost electrocatalysts.
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