AICHE JOURNAL
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2026
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IF 4.4
Aihemaiti Tuniyazi,Jing Li,Feng Li,Yi Zhang,Yating Yuan,Shuting Xi,Sheng Zhang,Shengping Wang
Electrocatalytic CO 2 reduction reaction (ECO 2 RR) faces limitations in conventional reactors due to high energy consumption, inefficient mass transport, and poor durability caused by ion-exchange membranes. Herein, we developed a membrane-free flow electrolyzer that dynamically decouples cathodic CO 2 -to-CO reduction from the anodic oxygen evolution reaction via a regenerative bromide cycle (Br − /BrO 3 − ). Operating at 216 mA cm −2 , the system achieves a record-low cell voltage of 1.85 V, maintains over 99% CO Faradaic efficiency, attains 32.9% single-pass CO 2 conversion, and reaches 71.9% energy efficiency (EE), with negligible degradation over 100 h of continuous operation. Operando spectroscopy reveals that local pH stabilization at 7.2 optimizes *CO/*H adsorption, thereby enhancing CO selectivity and EE. Techno-economic analysis shows a 60% lower power cost (111.8 vs. 277.79 $ ton −1 CO) vs. conventional systems. This work provides new insights into addressing persistent challenges in ECO 2 RR, including mass transfer limitations, carbonate formation, and anodic reaction mismatch.
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CHEMICAL ENGINEERING SCIENCE
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2026
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IF 5.1
Kangkang Li,Yulong Chen,Yong Cai,Yushi Jiang,Jiarong Huang,Zhuoran Zhang,Mengzhi Guo,Kaiqi Jiang
Amine scrubbing is the leading technology for decarbonizing, yet it faces critical challenges of high energy consumption and solvent degradation. Metal ions have long been recognized as detrimental to induce catalytic amine degradation, this study explores their potential by introducing metal additives into amine solutions to form a resilient metal-complexed amine system (MCAS). A comprehensive investigation of ten metals and sixteen amine formulations identified optimal metal-amine combinations, with Ni(II)-complexes exhibiting superior solubility, stability, and low toxicity. Experimental and modelling results confirmed that Ni(II)-complexes reduce CO 2 reaction heat by 12–41 % via dual synergistic mechanisms: shifting pathways from carbamate to bicarbonate formation, and chemical heat buffering via reversible complexation-decomplexation. Secondary amines like DEA benefited more enthalpy reduction due to carbamate instability and weaker metal-amine affinity, the blended solvent of Ni-PZ/AMP/AEEA achieved a 24.7 % reduction in reaction enthalpy with balanced CO 2 absorption kinetics and desorption efficiency. Furthermore, Ni(II)-MCAS exhibits superior chemical stability. EPR spectroscopy demonstrates that Ni-complexes stabilize radicals via the formation of metal–ligand–radical adducts, thereby suppressing degradation. DFT calculations further reveal that Ni-complexes modulate the electronic structure of amines, hindering hydrogen abstraction. Meanwhile, the formation energies of key degradation intermediates are elevated, leading to reduced reactivity. Importantly, kiloton-scale pilot validation demonstrates the practical applicability of Ni-PZ/AMP/AEEA, achieving a lower regeneration energy of 2.22 GJ/t CO 2 , compared to PZ/AMP/AEEA (2.35 GJ/t CO 2 ). These results highlight the role of MCAS in improving energy performance and solvent durability, providing a more systematic understanding to guide the design of solvents with enhanced industrial applicability.
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Nature Communications
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2026
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IF 18.1
Chen Qi-Fa,Wang Bingzheng,Chen Lei,Qiu Haoran,Chen Jiayi,You Fengqi,Wang Lei
The continuous decreasing in the levelized cost of renewable electricity has promoted the accelerated development of electrocatalysis, particularly electrochemical CO 2 reduction (CO 2 R) using dilute CO 2 concentrations (5-15%), which offers a sustainable pathway to convert waste CO 2 into fuels and chemicals. However, dilute CO 2 introduces substantial concentration overpotentials, leading to unsatisfactory selectivity and energy efficiency. Here, we develop effective approaches (pH control, amine addition, gas compression) to enrich the interfacial CO 2 availability, steering the CO 2 R selectivity towards the desired products. We further conduct techno-economic analysis and cradle-to-gate life cycle assessments to evaluate their economic and environmental performance. For instance, HCOOH production cost drops from 1.11 to 0.47 $ kg -1 , lower than the 0.58 $ kg -1 of the pure CO 2 scenario. Moreover, environmental burdens such as climate change and cumulative energy demand decrease by 38.2%-72.0% relative to the flue-gas scenario without these strategies. Overall, although variations in the electricity mix influence the absolute values reported in this study, our work provides critical implications and design principles for dilute CO 2 R.
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Molecular Catalysis
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2026
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IF 4.3
Hairen Tang,Shiyang Qin,Xiu Yu,Jiamiao Lu,Yubin He,Xudong Xiao,Haojie Song,Yanhong Zhang,Baojiang Jiang
Electron-rich CNNS and electron-deficient COFV induce a built-in electric field via Fermi-level equilibration. • PEI improves interfacial contact and strengthens charge transfer. • A metal-free Type-II heterojunction enables efficient directional charge migration. • Exceptional CO 2 photoreduction is achieved in pure water without sacrificial agents or metals. The development of efficient metal-free photocatalysts is of great importance for advancing solar-driven CO 2 conversion. Graphitic carbon nitride (g-C 3 N 4 ) has attracted extensive attention due to its unique electronic structure and excellent stability; however, its photocatalytic efficiency is severely limited by rapid photogenerated charge carrier recombination. Herein, we construct a metal-free COFV/CNNS heterojunction by exploiting the electronic disparity between electron-rich carbon nitride nanosheets (CNNS) and an electron-deficient π-conjugated covalent organic framework (COFV). A polyethyleneimine (PEI)-mediated surface modification strategy is employed to regulate interfacial assembly and enhance interfacial contact between the two components. The intimate heterointerface induces interfacial charge redistribution driven by the intrinsic electronic disparity between CNNS and COFV, leading to the formation of a built-in electric field at the interface through Fermi-level equilibration and electronic coupling. This internal electric field, together with the strong interfacial interaction, promotes efficient separation and directional migration of photogenerated charge carriers, thereby suppressing recombination and significantly enhancing photocatalytic performance. The optimized COFV/CNNS-60 composite exhibits a CO evolution rate of 14.8 times that of pristine CNNS and 3.9 times that of COFV under visible-light irradiation (λ ≥ 420 nm) in pure water without any sacrificial agents. This work provides a general strategy for constructing high-performance metal-free photocatalysts via interfacial electronic regulation and interface engineering, offering new insights into sustainable solar-to-fuel conversion. Download: Download high-res image (407KB) Download: Download full-size image
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2026
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IF 4.4
Mengyuan Zhao,Lulu Ren,Yameng Li,Xin Lu,Jingwen Meng,Xiaodi Liu,Xin Li,Fengyun Su,Zhonghua Fu,Xiaoli Jin,Haiquan Xie
A Synergistic strategy that integrates the intrinsic polarization field with heterojunction interfacial engineering is demonstrated for boosting photocatalytic CO 2 reduction. In the engineered Bi 4 O 5 Br 2 /Nb 2 O 5 heterojunction, a structure has not been previously reported for CO 2 photoreduction to date, the intrinsic polarization field of Bi 4 O 5 Br 2 facilitates initial charge separation within the bulk phase. The type-ii interfacial field drives the transfer of separated electrons toNb 2 O 5 , achieving effective spatial separation of carriers. This efficient charge separation promotes surface reactions, as evidenced by in situ diffuse reflectance infrared fourier transform spectroscopy (DRIFTS), which reveals accelerated formation and transformation of key intermediates (*CO 2 , *COOH and *CHO) along the reaction pathways toward CO and CH 4 . Using ultrapure water as the proton source, the CO and CH 4 production rates of the optimal composite reach 4.6 and 3.7 μmol g −1 h −1 , respectively, which are 2.0 and 4.6 times higher than those of pristine Bi 4 O 5 Br 2 . In contrast to conventional heterojunction strategies that focus solely on interfacial band engineering, this work simultaneously leverages the intrinsic properties of bulk materials, offering a new design paradigm for efficient CO 2 photoreduction.
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ENERGY & FUELS
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2026
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IF 6
Lefei Cao,Fei Qi,Chengfan Fu,Ge Xu,Nan Zhang,Yayun Pu,Xiaosheng Tang,Qiang Huang
Although dielectric barrier discharge (DBD) plasma represents a promising technology for CO2 conversion, its standalone application remains limited by low conversion efficiency, which could be improved via filling a suitable photocatalyst into the plasma reactor. In this paper, the synergistic effect of discharge plasma and Bi12O17Cl2@Cs2SnCl6–Sb0.35 photocatalyst was studied, achieving efficient carbon dioxide conversion. With the help of a photocatalyst, DBD plasma successfully realized the conversion of CO2 and water to CO, methanol, and ethanol. Compared with Cs2SnCl6–Sb0.35, Bi12O17Cl2-10@Cs2SnCl6–Sb0.35 increased methanol and ethanol production by 186 and 80%, respectively. Meanwhile, the conversion of carbon dioxide increased significantly with the presence of water in the plasma-photocatalyst system, achieving a conversion ratio of 35.6%. This boost is attributed to the enhancement of the surface conductivity of the photocatalyst during the plasma discharge, which in turn optimizes the charge transfer process. This paper provides a new idea and a promising technical roadmap for the resource utilization of CO2, which exhibits scientific significance and application potential.
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Nature Communications
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2026
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IF 18.1
Yin Chenxu,Sun Zhecheng,Tang Kunlin,Zou Weixin,Wan Haiqin,Liu Zhao-Qing,Dong Lin
Photocatalytic reduction of CO 2 to natural gas using water vapor is a promising strategy for carbon recycling and renewable energy storage. However, the selectivity of current catalysts still remains a big challenge. Herein, we construct IrCu alloys on TiO 2 nanosheets to promote photocatalytic CO 2 to methane with 98.6% selectivity and 7.9% quantum efficiency at 365 nm under non-sacrificial ambient conditions. The performance is competitive with most other reported metal-based photocatalysts. Experimental and theoretical calculations demonstrate that the intensive H 2 O adsorption on Ir/TiO 2 hinders *H transfer, inevitably generating the H 2 by-product. Conversely, hydrophobic Cu effectively optimizes the interfacial hydrogen-bond network on IrCu/TiO 2 , predominantly in H-down configurations for H 2 O adsorption on the asymmetric charge-polarized Cu δ+ -Ir δ- structure, which facilitates the kinetic migration of dissociated *H to *CO-Cu sites, resulting in the reduced energy barrier for the key *CHO intermediate. This finding enables high CH 4 selectivity on IrCu/TiO 2 , deepening our understanding of gas-solid interfacial water vapor in the enhanced natural gas synthesis.
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PubMed
高影响因子
Journal of Photonics for Energy
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2026
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IF 2.5
Pengyu Fei,Yun Li,LingLing Jiao,Fan Cao,Zhouze Chen,Hongbin He,Ruoxuan Peng,XingYu Zhan,Jiancheng Zhou,Yitao Si,Naixu Li
Photothermal-assisted photocatalysis, which couples localized thermal energy with photogenerated charge carriers to overcome thermodynamic and kinetic limitations, has emerged as an effective strategy for solar-driven CO2 reduction. Herein, nanoflower-like NiO/ZnO p–n heterojunction spheres were rationally constructed via a simple hydrothermal calcination method to achieve efficient concentrated photothermal-assisted CO2 reduction. The unique nanoflower morphology provides abundant interfacial contact between NiO and ZnO, while the formation of the p–n heterojunction establishes an internal electric field that suppresses electron-hole recombination. Under concentrated irradiation (4.31 W·cm−2), the photothermal coupling effect reduces the apparent activation energy and enables the NiO/ZnO photocatalyst to deliver CO and CH4 production rates of 51.78 and 15.96 μmol·g−1·h−1, which are 7.92 and 9.61 times higher, respectively, than those obtained under nonconcentrated illumination. Photoelectrochemical measurements and in situ DRIFTS further reveal that the built-in electric field facilitates directional charge transfer from ZnO to NiO, thereby promoting CO2 adsorption and activation. We demonstrate an efficient photothermal-coupling strategy to construct high-performance catalysts for artificial photosynthesis and solar-to-fuel conversion.
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INORGANIC CHEMISTRY
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2026
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IF 4.6
Hongxiang Jin,Xiaochuan Deng,Rong He,Lingyu Xie,Xue Wang,Han Yan,Aiping Zhang,Xiaofang Feng,Tao Chen,Wenkun Zhu
The conversion of CO2/H2O into valuable chemicals with nonthermal plasma (NTP) under mild conditions represents a promising strategy, whereas the quenching effect and side reactions caused by H2O seriously restrict its efficiency. Herein, we propose a surface microenvironment modulation strategy by confining phosphomolybdic acid (PMA) within UiO-66 to construct a highly hydrophilic PMA/UiO-66 catalyst for plasma-catalytic CO2 conversion in a dielectric barrier discharge system. Theoretical calculations and experimental results confirm that the abundant exposed oxygen atoms in PMA/UiO-66 can form a hydrogen-bonding network with H2O molecule, which effectively promotes the enrichment and activation of H2O on the catalyst surface and suppresses the quenching effect of bulk H2O molecules on the plasma-induced dissociation of CO2. Meanwhile, the hydrogen-bonding network acts as an electron-trapping center and proton transport channel, lowering the free energy barrier for CO2-to-*COOH step, thereby accelerating the reaction kinetics of CO2 conversion. Under optimal energy efficiency conditions for NTP-catalyzed CO2 conversion, the PMA/UiO-66 system achieves a CO2 conversion of 17.78%, which is approximately 5 times greater than that of the plasma-only system. The study on the regulation of the catalyst surface microenvironment offers valuable insights for designing high-performance catalysts for plasma-catalytic CO2 conversion.
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APPLIED SURFACE SCIENCE
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2026
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IF 6.6
Jibiao Wang,Jiansen Wang,Lingyun Yang,Houyu Zhu,Pornthip Tongying,Yuanxing Wang
Oxide-derived Cu nanowire arrays were developed for electrochemical CO 2 reduction. • Cu nanowire arrays are capable of producing syngas with a wide range of H 2 /CO ratios. • The tunable selectivity of catalysts was attributed to the grain boundaries in Cu. Electrochemical reduction of CO 2 to value-added fuels and chemical feedstocks, such as syngas, stands as an appealing solution for energy and environmental sustainability. Currently, it suffers from a lack of catalysts with good activity and selectivity. Herein, we have synthesized a series of oxide-derived Cu nanowire arrays (NAs) as catalysts for electrochemical CO 2 reduction. Copper oxides NAs were first synthesized by thermal oxidation and then electrochemically reduced. By adjusting the annealing temperatures, the obtained Cu NAs are capable of reducing CO 2 and H 2 O to produce syngas with a wide range of H 2 /CO ratios (from 2.5:1 to 0.7:1) at a low overpotential. First-principles calculations confirmed that the enhancement of CO 2 reduction and suppression of hydrogen evolution were attributed to grain boundaries in the Cu NAs. This research demonstrates a promising strategy for the development of Cu-based catalysts in tunable syngas production. Download: Download high-res image (187KB) Download: Download full-size image
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Yanni Lang,Dongfeng Hong,Rongze Ma,Haoqiang Zhang,Liang Xu,Xinye Zhao,Dan Wu,Yongjin Li,Dacheng Zhou,Zhiguo Song,Yugeng Wen,Yong Yang,Jin Han,Jianbei Qiu
The construction of chiral materials has always been a research hotspot in the field of non-chiral nanomaterials. By introducing chiral destructive agents, materials are endowed with chiral nanostructures, which can be used in the field of photocatalysis. Au nanoparticles (Au NPs) are a typical photosensitizer capable of producing surface plasmon resonance (SPR) effects, producing CO and CH 4 in photocatalytic CO 2 reduction. We suggest that the SPR effect of the photocatalyst (D-BiOBr/Au) for Au NPS deposition of nonchiral bismuth bromide oxide nanomaterials can enhance the photocatalytic CO 2 reduction by enhancing spin-polarized electrons. It is worth noting that D-BiOBr/Au chiral materials enhance spin-polarized electrons due to SPR effect, and their photocatalytic CO 2 reduction performance is significantly better than D-BiOBr and original BiOBr without SPR effect. The CO yield of D-BiOBr/Au is 24.39 μmol/g h −1 , which is 2.02 times of D-BiOBr and 2.43 times of BiOBr, respectively. The mechanism of photocatalytic CO 2 reduction was further studied by FDTD simulation. The reason for the improved photocatalytic CO 2 reduction efficiency of D-BiOBr/Au is the increase of spin-polarized electrons due to the SPR effect, thus prolonging the carrier lifetime and promoting spin-polarized electron-hole separation. The results show that enhancing spin-polarized electrons through SPR effect is an effective strategy to improve photocatalyzed CO 2 reduction in photocatalyzed semiconductors.
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Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Ziyan Liu,Junrong Chen,Yuanlan Wang,Wenqing Zhang,Wenlei Wang,Jing Wang
The photocatalytic reduction of CO 2 to CO is often constrained by suboptimal visible-light harvesting, interfacial recombination losses, and durability under repeated cycling. Here we design a Bi–BiOBr@CNF architecture that integrates metallic Bi (for plasmon-assisted excitation and interfacial electron transfer), oxygen/bromine vacancies (for CO 2 adsorption/activation), and a conductive CNF network (for dispersion and transport). Photoelectrochemical characterizations elucidate the synergistic mechanism. Under visible light, the catalyst delivers CO as the single detectable product with high selectivity; cycling tests reveal performance decay that is mechanistically linked to defect evolution, and a moderate-temperature regeneration restores activity. The results elucidate the respective roles of Bi 0 , O V , Br V , and the CNF scaffold within an integrated mechanistic framework, and indicate a viable strategy for durable photocatalytic reduction of CO 2 to CO.
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