ADVANCED FUNCTIONAL MATERIALS
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2024
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IF 18.5
Zhenyao Li,Wei Wei,Xuli Hu,Zhen Zhang,Yangshun Hu,Yushan Wu,Yao Wang,Junchen Xu,Mingyue Ding
While engineering lattice strain has been proven effective in enhancing the electrochemical CO 2 reduction performance of a catalyst, the correlation between strain effect and the intrinsic catalytic mechanism has remained elusive. Herein, a photolithography-inspired method is proposed to regulate Cu(111) lattice strain. By irradiating the photosensitive Cu(Acac) sol–gel, Acac chelate bond undergoes π→π * electronic transition, and the ring-closed Cu(Acac) decompose into the stabilized Cu(Acac) mesh which presents as nanospots embedded onto the surface of the Cu cluster. The photoinduced nanospots serve to exert compressive strain to the Cu(111) lattice in which the lattice distance is reduced by 5.7–11.4%. Herein, the catalyst with 11.4% lattice compression exhibits enhanced C 2 H 4 production capabilities, reaching a maximal Faradaic efficiency of 57.00%, and a high partial current density of 456.01 mA cm −2 . Theoretical calculations reveal that the compressed Cu(111) lattice exhibits reduced surface energies, leading to a significant drop in the C─C coupling reaction free energy from 1.16 eV over the pristine lattice, to 0.57 eV over the 10% compressed lattice. Additionally, the 10% compressed lattice facilitates spontaneous *O splitting immediately after OC─CHO coupling which leads to the generation of C 2 H 4 -favoring *CCH intermediate.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2024
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IF 5.9
Chengzhi Liu,Yanqi Zou,Kunmei Su,Zhenhuan Li
The emission of significant amounts of CO 2 from human industry has caused severe environmental damage, necessitating effective CO 2 capture methods for sustainable development. Membrane technology stands out as one of the most effective and economical solutions. In recent decades, polymer membranes have been recognized for their viability in gas separation applications. Aliphatic polycarbonates (APCs) are particularly notable due to their high chain segment flexibility, degradability, ease of processing, and the presence of carbonate groups, which enhance their affinity for CO 2 . This study uses a one-pot melt polycondensation process to synthesize three high-molecular-weight APCs: poly(1,4-butylene carbonate) (PBC), poly(1,5-pentamethylene carbonate) (PPC), and poly(1,6-hexamethylene carbonate) (PHC) from dimethyl carbonate and various diols. To improve the mechanical properties of the APC separation membranes, capping modification was applied. The molecular weights of PBC, PPC, and PHC were 6.48 × 10 4 g/mol, 4.78 × 10 4 g/mol, and 5.76 × 10 4 g/mol, respectively. These membranes were prepared by the evaporative solvent method. The PHC membrane demonstrated a CO 2 permeability of 20.84 Barrer and a CO 2 /N 2 selectivity of 22.24 at 35 °C under 0.1 MPa, approaching Robeson’s upper bound and indicating substantial potential for application.
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C-Journal of Carbon Research
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2024
·Vol. 10
·期 3
·62
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IF 3.9
Xuexin Yuan,Qiqi Zhou,Yu Chen,Hai-Jian Yang,Qingqing Jiang,Juncheng Hu,Cun-Yue Guo
In the present work, inexpensive and commercially available diethyltriamine pentaacetic acid (DTPA) was used as an initiator to catalyze the N-formylation reaction of CO2with amines via the construction of C-N bonds in the presence of xanthone as the photosensitizer and PhSiH3as the reducing agent. After a systematic study of various factors, the optimal conditions for the photocatalytic reaction were obtained: 2.5 mmol of amine, 2.5 mmol of PhSiH3, 10 mol% of DTPA, 20 mol% of xanthone, 1 mL of dimethylsulfoxide (DMSO), atmospheric pressure, and 35 W UV lamp irradiation for 48 h. Under the optimal conditions, the catalyst system afforded high performance for the N-formylation of amines (primary and secondary amines) and CO2, and the yields of the N-formylated products of dialkylamines were above 70%. Further studies exhibit that the catalytic system has a wide scope of substrate applications. For various alicyclic secondary amines, heterocyclic secondary amines, aliphatic primary amines, and aromatic primary amines, the corresponding N-formylation products can be obtained efficiently. In addition, the catalyst can be recycled by simple precipitation and filtration. After five cycles of recycling, there was no significant change in the catalytic and structural properties of DTPA. Finally, a possible reaction mechanism is proposed.
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APPLIED SURFACE SCIENCE
·
2024
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IF 6.3
Yingzi Hu,Yan Zhu,Xi He,Ya-Nan Feng,Fei-Fei Chen,Yan Yu
Two-dimension nanosheets are ideal photocatalysts for CO 2 reduction due to their high exposure of active sites and short charge transfer pathway. However, 2D photocatalysts have a tendency to agglomeration, thus compromising the performance of photocatalytic CO 2 reduction. Trees, one of the most important plants for photosynthesis, have a unique “leaf-on-branch” structure. This unique two-dimension/one-dimension (2D/1D) configuration maximizes the adsorption of CO 2 molecules and light harvesting. Herein, a tree-inspired semiconductor-on-ceramic 2D/1D heterostructure for efficient photocatalytic CO 2 reduction is reported. The cobalt silicate (CoSi) nanosheets (∼0.68 nm) are in situ grown on the surfaces of hydroxyapatite (HAP) nanowires, creating a well-defined 2D/1D hierarchical structure. The vertical alignment of ultrathin CoSi nanosheets on the HAP nanowires effectively suppresses their agglomeration, leading to a large BET surface area (106.45 m 2 /g) and excellent CO 2 adsorption (8.00 cm 3 g −1 ). The results of photoelectrochemical characterization demonstrate that the 2D/1D hierarchical structure is powerful to expedite charge transfer. As a result, the gas generation rate of CO is as high as 28780 μmol g −1 h −1 over the CoSi-on-HAP 2D/1D heterostructure. In addition, the electron transfer mechanism and reaction pathways of CO 2 reduction are revealed by in situ irradiated XPS and in situ DRIFT spectra.
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CHEMICAL ENGINEERING JOURNAL
·
2024
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IF 13.3
Fayi Jin,Xiaoli Yang,Jia Yang,Yang Lei,Wenfan Xu,Wei Jiang,Zhen Ma,Gemeng Liang,Haoxi Ben,Xingyun Li
Oxygen vacancies in oxides are core parameters determining the catalytic performance in various reactions. This study investigated the influence of oxygen vacancies of MoO x catalysts on the reverse water gas shift (RWGS) reaction to gain a deep insight into the structure–function relationship. A distinct volcano-shaped trend was observed among MoO x catalysts with different amounts of oxygen vacancies. Through comprehensive characterizations and steady-state kinetic analysis, an optimal concentration of oxygen vacancies was identified to not only facilitate the adsorption and activation of CO 2 but also restrain the formation of by-product CH 4 . In-situ characterizations combined with DFT calculations uncovered a formate-involved reaction pathway over the oxygen vacancies structured MoO x catalyst, with the hydrogenation of formate identified as the rate-determining step. These findings not only showcase the potential of Mo-based oxides in CO 2 hydrogenation reactions but also provide fundamental insights into the role of oxygen vacancies in shaping catalytic behavior.
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Small
·
2024
·Vol. 20
·期 37
·2401530
·
IF 13
Zezhong Xie,Qiushi Wang,Hao Yang,Jin Feng,Jian Chen,Shuqin Song,Changgong Meng,Kun Wang,Yexiang Tong
The unavoidable and unpredictable surface reconstruction of metallic copper (Cu) during the electrocatalytic carbon dioxide (CO 2 ) reduction process is a double-edged sword affecting the production of high-value-added hydrocarbon products. It is crucial to control the surface facet reconstruction and regulate the targeted facets/facet interfaces, and further understand the mechanism between activity/selectivity and the reconstructed structure of Cu for CO 2 reduction. Based on the current catalyst design methods, a facile strategy combining chemical reduction and electro-reduction is proposed to achieve specified Cu(111) facets and the Cu(110)/(111) interfaces in reconstructed Cu derived from cuprous oxide (Cu 2 O). The surface facet reconstruction significantly boosted the electrocatalytic conversion of CO 2 into multi-carbon (C 2+ ) products comparing to the unmodified catalyst. Theoretical and experimental analyses show that the Cu(110)/(111)s interface between Cu(110) and a small amount of Cu(111) can tailor the reaction routes and lower the reaction energy barrier of C–C coupling to ethylene (C 2 H 4 ). The work will guide the surface facets reconstruction strategy for Cu-based CO 2 electrocatalysts, providing a promising paradigm to understand the structural variation in catalysts.
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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Liju Bai,Shuai Wang,Xiaotong Jiang,Zixuan Hao,Tejraj M. Aminabhavi,Helei Liu
CO 2 capture is crucial for achieving carbon emission reduction targets. At present, porous carbon is regarded as an effective CO 2 capture material. However, the limited adsorption capacity restrains its practical application, due to the insufficient adsorption sites. In this work, N-doped porous carbon derived from heterogeneous polymers is employed to investigate efficient CO 2 capture. Porous carbon was prepared by pyrolyzing KOH activated melamine-phenolic resin-based heterogeneous polymers. By optimizing pyrolysis temperature, the derived carbon material exhibits a high specific surface area (1274.4 m 2 /g), an abundant microporous structure (0.823 nm in pore diameter), and a substantial N retention (5.22 wt%). These characteristics synergistically enhance its CO 2 adsorption performance. Consequently, an exceptional CO 2 capture capacity of 100.8 mL/g (~4.5 mmol/g) at 25 °C and 1 bar was obtained, surpassing the most reported porous carbon materials. Besides, the prepared porous carbon demonstrates outstanding CO 2 /N 2 selectivity (25.0) and rapid adsorption kinetics, fitting the pseudo-first-order model (R 2 = 0.997) with reaching the equilibrium in 60 min. The calculated low adsorption heat (~25 kJ/mol) confirms physical adsorption mechanism, further supported by excellent renewability and cyclic stability over the five consecutive PSA cycles. Comparative analysis highlights its superior N efficiency and CO 2 capture performance relative to conventional porous carbons. These findings not only elucidate the critical role of the pore structure and N-doped in CO 2 adsorption validating the potential of the material for scalable industrial applications, offering a sustainable pathway for carbon capture technologies.
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Science Advances
·
2025
·Vol. 11
·期 35
·
IF 12.5
Zhiyong Yu,Qing Yao,Wei An,Hangjun Xu,Jiaqi Su,Juan Wang,Ying Zhang,Huile Jin,Yonggang Feng,Xiaoqing Huang
Electrocatalytic CO 2 reduction (ECR) to formic acid faces challenges in separating and purifying a formate-electrolyte mixture. In situ utilization of this mixture presents a promising yet underexplored solution. Here, we report the synthesis of Bi x Pd 1− x Te nanocrystals (NCs) via a microwave-assisted cation topological exchange approach, enabling the precise tuning of surface oxygen affinities to simultaneously optimize the ECR and catalytic transfer hydrogenation (CTH) of phenol. Optimized Bi 0.1 Pd 0.9 Te NCs achieve a 92% formate Faradaic efficiency at −0.9 volts versus reversible hydrogen electrode and a production rate of 860 millimoles per hour per gram of catalyst at 100 milliamperes per square centimeter. This formate-electrolyte mixture serves as an effective hydrogen donor, enabling 98% selectivity toward cyclohexanone in phenol hydrogenation. Mechanistic studies show uniformly dispersed Bi sites create an oxygen affinity gradient, enhancing *OCHO adsorption for formate production and promoting noncoplanar phenol adsorption for selective cyclohexanone formation. This work pioneers synergistic ECR-CTH integration, establishing an innovative CO 2 valorization and biomass upgrading strategy.
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ADVANCED FUNCTIONAL MATERIALS
·
2025
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IF 19
Shenzhen Cong,Si Sun,Yijing Zhang,Ming Wang,Zhehua Jia,Youhua Zhao,Huan Pang
Metal–organic framework (MOF) membranes offer a wide range of applications, including simultaneous hydrogen generation and decarbonization. The permselectivity of gas molecules can be considerably increased by optimizing the oriented of MOF membranes, and it is possible to construct MOF membranes with high permeance and high selectivity. Here, chelation-assisted interfacial growth is used to prepare ZIF-L membranes for H 2 /CO 2 separation. The growth rate of the ZIF-L crystal plane is regulated by optimizing the interface Zn 2+ diffusion, and a ZIF-L membrane with preferred orientation is constructed for efficient separation of H 2 /CO 2 . The optimized ZIF-L membrane has an H 2 permeance of over 2000 GPU, and the H 2 /CO 2 selectivity exceeds 30. Additionally, the prepared ZIF-L membrane exhibits outstanding operating stability and tolerance, making it a promising candidate for industrial applications.
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Cell Reports Physical Science
·
2025
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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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Journal of Energy Chemistry
·
2025
·
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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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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