Science China-Chemistry
·
2026
·
IF 9.8
Wang Yi-Rong,Yue Ming,Zhang Jia-Li,Xia Yuan-Sheng,Yang Le,Li Run-Han,Shi Jing-Wen,Li Qi,Chen Yifa,Li Shun-Li,Lan Ya-Qian
The development of electrocatalytic CO 2 reduction reaction (eCO 2 RR) in upgrading CO 2 into valuable products affords a substantially untapped opportunity to simultaneously achieve a circular economy and tackle environmental problems. However, the current challenges of this process lie in the low efficiency of eCO 2 RR, less explored product-upgrading systems, as well as the unmet while key electrocatalysts. Here, we develop a parallel-integrated eCO 2 RR cascade catalysis system based on a kind of covalent organic framework (Bpy-COF-Co) electrocatalyst with mesoporous nanosphere morphology that enables efficient cascade conversion of CO 2 into carbonyl compounds with high yields. In the parallel eCO 2 RR modules, the specially designed Bpy-COF-Co with the advantages of high porosity, mesoporous nanosphere morphology and active Co sites presents a remarkable CO generation rate with a superior FE CO (∼100%) and thus-generated CO can be simultaneously utilized in a series of backend carbonylation reactions ( e.g. , amino-carbonylation, carbonylative Suzuki coupling, alkoxy-carbonylation and phenoxy-carbonylation). Noteworthy, this system can achieve gram-scale generation of valuable products like pesticide diethyltoluamide (1.81 g, 94.7% yield).
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ACS Sustainable Chemistry & Engineering
·
2026
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IF 7.6
Sun Mingyang,Hu Ziyan,Liu Yilang,Lv Chenyan,Zhang Tuo,Zhao Guanghua,Zang Jiachen
Efficient noble-metal-free photosynthesis systems for CO 2 conversion based on earth-abundant elements have been largely unexplored. On the other hand, large quantities of bovine blood as waste byproducts during meat processing pose environmental challenges. To address these concerns, herein we report a biomimetic photocatalytic platform constructed by hemoglobin, a major component in bovine blood, which structurally and functionally emulates the fibrous chloroplasts of Spirogyra . Under denaturing conditions, hemoglobin molecules self-assemble into heme-containing amyloid-like fibrils, in which the intrinsic heme groups serve as visible-light photosensitizers. Subsequently, iron-based catalytic cores are uniformly deposited along the protein fibrils, generating a hierarchical architecture that integrates heme as a light-harvesting domain and iron cores as catalytic functionalities within a single scaffold. This spatially organized system effectively shortens electron transfer distances and promotes interfacial charge migration. Consequently, the as-prepared biomimetic assembly exhibits efficient visible-light-driven CO 2 reduction to formic acid with high activity and selectivity as compared to conventional homogeneous systems. Notably, this work not only provides a noble-metal-free strategy for constructing integrated photocatalytic systems but also demonstrates a viable pathway for transforming biological waste into high-value functional materials.
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Carbon Capture Science & Technology
·
2026
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IF 10.2
Ali A. AL-Thuraya,Wen He,Jingcheng Du,Pengjia Dou,Qian Sun,Ayan Yao,Xuan Ding,Daijun Meng,Jiangtao Liu
Polymeric membranes for CO 2 capture often face a trade-off between permeability and selectivity. Here, crown ethers were introduced as molecular shuttles for CO 2 transport by in situ encapsulation within ZIF-8 nanocages. Three crown ethers (18-crown-6 (18C6), diaza-18-crown-6 (DAC), and dibenzo-18-crown-6 (DBC)) were incorporated into ZIF-8 during crystallization and then used as low-loading fillers in Pebax mixed-matrix membranes. Structural characterization by XRD, FTIR, SEM/EDS, and BET confirmed that ZIF-8 crystallinity was preserved, while pore volume, linker rotation, and filler dispersion were effectively tuned. These modifications narrowed transport pathways and strengthened polymer–filler interactions, improving CO 2 separation performance. At an optimal loading of 1 wt% 18C6@ZIF-8, the membrane doubled CO 2 permeability relative to neat Pebax and increased CO 2 /N 2 selectivity from 55.5 to 85.8, surpassing the 2008 Robeson upper bound. The membrane also maintained stable performance under feed pressures up to 20 bar and exceeded the 2019 Robeson upper bound. Mixed-gas testing showed a CO 2 permeability of 158.3 Barrer and CO 2 /N 2 selectivity of 66.0, outperforming neat Pebax. Transport analysis revealed that the enhancement mainly arose from improved diffusion selectivity, with a minor contribution from solubility selectivity. Among the fillers, 18C6@ZIF-8 provided the best permeability–selectivity balance, demonstrating a promising strategy for advanced CO 2 -selective mixed-matrix membranes. This approach paves the way for the development of next-generation mixed-matrix membranes (MMMs) with enhanced performance for CO 2 capture and a range of other gas-separation applications.
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Molecular Catalysis
·
2026
·
IF 4.3
Minghao Geng,Jiahao Li,Zhengze Li,Meng Sui,Fashe Li,Hua Wang,Zhiyu Hua
Fe-modulated Cu-ZnO CeO 2 catalysts were synthesized via sol-gel method. • Moderate Fe doping suppressed CuO growth and improved Cu dispersion. • Fe tuned the interface and oxygen defects to balance reducibility. • Fe10-CZCe achieved 14.5% CO 2 conversion with high methanol selectivity. • The promotion by Fe stems from interfacial regulation, not new phases. Copper-based catalysts have been widely applied in methanol synthesis from CO 2 hydrogenation. Yet efficient operation at an industrially relevant level remains challenging. The use of CO 2 as a carbon source is still limited by difficult molecular activation and by imperfect interfacial matching. Here, a series of Fe-doped Cu-ZnO CeO 2 catalysts was prepared by a sol-gel route. The influence of Fe content on phase structure, surface electronic environment, reduction behaviour, CO 2 adsorption characteristics and catalytic performance was examined systematically. Fe incorporation did not change the fundamental phase composition of CuO and CeO 2 . It did, however, strongly affect Cu dispersion, the near-surface defect environment of CeO 2 , and the electronic structure of the interface. Moderate Fe addition suppressed CuO crystallite growth, improved Cu dispersion, and produced a more concentrated reduction profile with a more suitable distribution of CO 2 adsorption strength. Excess Fe enhanced defect-related signals and high-temperature adsorption, but also increased interfacial perturbation, which was unfavourable for the further conversion of intermediates. At 3 MPa and 260 °C, Fe10-CZCe showed the best overall performance, giving a CO 2 conversion of 14.5% together with high methanol selectivity and the highest methanol space-time yield. The beneficial role of Fe is therefore linked to reconstruction of the Cu-ZnO CeO 2 interface, which promotes a more effective balance between CO 2 adsorption, activation and hydrogenation. These findings provide a useful perspective for compositional tuning and interface design in Cu-based catalysts. Download: Download high-res image (231KB) Download: Download full-size image
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Journal of the American Chemical Society
·
2026
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IF 16.6
Hou Tianfeng,Tang Tongming,Feng Yuhua,Yang Qingzhuoma,Wei Jinman,Wang Lin,He Donghao,Chen Zhen,Hu Jianjun,Zeng Cuiping,Yu Tao,Wang Bo
Carbon-negative biomanufacturing is essential for global
sustainability.
Artificial photosynthesis based on material-microbe hybrid systems
holds promise but suffers from inefficient energy supply, phototoxicity,
abiotic–biotic incompatibility, and limited product spectrum.
Here, we present artificial photosynthetic hydrogel microspheres (APHM)
as a versatile platform for efficient and programmable CO 2 valorization. Within an alginate/carboxymethyl cellulose hydrogel
matrix, spatial compartmentalization integrated a COF/Pt/Cr 2 O 3 photocatalyst (for in situ hydrogen evolution) and
a light-shielded acetogen ( Acetobacterium woodii ) in a tailored bifunctional medium, enabling CO 2 -to-acetate
conversion. The system operated stably under high-intensity illumination
(60 mW cm –2 ), achieving a near-stoichiometric H 2 -to-acetate coupling efficiency of 88.85%. The resulting acetate
served as a well-defined carbon hub, enabling seamless interface with
engineered yeast for programmable synthesis of diverse products, including
glucose (316 mg L –1 ), myo -inositol
(64 mg L –1 ), glucosamine (24 mg L –1 ), sucrose (609 mg L –1 ), and starch (256 mg L –1 ). Overall, this work presents a universal, efficient
route to versatile solar-to-chemical synthesis.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2026
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IF 6.7
Tianyi Li,Xing Liu,Yudong Li,Gongwei Tian,Haiyue Yang,Chengyu Wang
To overcome the limitations of traditional binary sulfide photodegradation and charge recombination, ternary metal sulfide solid solutions provide a promising solution through atomic-level bonding reconfiguration, continuous electron distribution, and the synergy of dual metal sites. In the present study, a Cu 3 SbS 4 solid solution photocatalyst was successfully synthesized via a hydrothermal approach, exhibiting superior performance in the photoreduction of CO 2 , demonstrating high selectivity for the conversion of CO 2 to CO and CH 4 , with yields of 1.8083 mmol g –1 and 0.4232 mmol g –1 , respectively, over a 5-hour reaction duration, alongside excellent cycling stability. Combining in situ spectroscopy with DFT calculations, the enhanced photocatalytic activity of Cu 3 SbS 4 stems from the cooperative bonding effect within its molecular framework. Specifically, the Cu–S bonds form a continuous low-energy barrier path, facilitating electron localization and inhibiting interphase carrier recombination, while the Sb–S bonds construct local active sites on the surface, facilitating CO 2 adsorption and activation. The Electron Localization Function (ELF) analysis indicates that this solid solution overcomes the discontinuous, island-like electron distribution characteristics in the binary system, forming a uniform and continuous network of electron localization, significantly reducing the in situ recombination centers. The synergistic action of the bimetallic (Cu/Sb) sites reduces the key reaction energy barriers, and local lattice distortion exposes high-activity surface sites. Additionally, the elongation of the Cu–S bonds increase the oxidation energy barrier of sulfur, effectively alleviating photodegradation. This study provides atomic-scale evidence for the rational design of bonding cooperation in multi-component sulfide solid solution photocatalysts.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2026
·Vol. 65
·期 34
·18159-18168
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IF 3.9
Ren Xuping,Zhao Zijiang,Long Yanhui,Zhang Wenjun,Wang Jun,Zhang Hao
Developing efficient catalysts for
CO 2 hydrogenation
to methanol remains a challenge due to the inherent trade-off between
activity, selectivity, and cost. Herein, a series of metal-promoted
Cu catalysts (Zr, Zn, Ga) were synthesized via a ligand-modulated
oxalate coprecipitation strategy using malachite-derived CuO as the
precursor, enabling a low-cost and sustainable catalyst design. Among
these, the ZrO 2 /Cu catalyst (Zr/Cu = 14:86) exhibits the
optimal performance, delivering a CO 2 conversion of 13%
and a methanol space-time yield (STY) of 280.1 g MeOH ·kg cat –1 ·h –1 at 280 ° C
and 3.0 MPa, together with excellent long-term stability. Characterization
results suggest that highly dispersed Zr species effectively suppress
Cu particle agglomeration while generating abundant surface oxygen
vacancies (O V , 43.5%). Mechanistic studies indicate that
Zr incorporation induces strong electronic metal–support interactions
(EMSI), leading to the formation of electron-rich Cu 0 /Cu + sites. These sites act cooperatively with O V ,
where the former facilitates H 2 dissociation and the latter
promotes CO 2 adsorption and activation. Such synergistic
effects favor the formate-mediated pathway while suppressing the competing
reverse water–gas shift reaction. This work not only demonstrates
a high-performance catalyst derived from natural minerals but also
provides insights into the atomic-level synergy between electron-rich
metal sites and surface defects, offering a viable strategy for the
rational design of efficient catalysts for CO 2 hydrogenation.
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Green Chemical Engineering
·
2026
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IF 11.9
Xin-Yi Yang,An-Guo Wu,Fang-Yu Yu,Li-Feng Xu,Guang-Rui Liu,Hong-Ru Li,Liang-Nian He
In this work, a “CO 2 capture and ex situ utilization” strategy was proposed by combining calcium looping and a subsequent cycloaddition reaction. In the calcium looping step, the CaO-based sorbent was prepared from bulk industrial solid waste, i.e., carbide slag as the calcium source and blast-furnace slag as the dopant. Both wet mixing and sol-gel methods were explored in this study. Among them, the sorbent synthesized via the sol-gel route with sucrose as a complexing agent showed improved cyclic performance. This improvement is presumably attributable to the sol-gel method's ability to enhance the distribution of blast furnace slag and optimize the sorbent's pore structure. By further regulating sorbent preparation parameters such as the mass ratio of carbide slag to blast furnace slag, the sucrose amount, and the calcination temperature and time, the optimal sorbent was obtained with an initial CO 2 uptake of 0.552 g CO 2 /g sorbent at 740 o C. Furthermore, the CO 2 uptake was still retained at 92% even after 10 cycles. The CO 2 released from Ca-looping ex situ reacted with propylene oxide (PO) to afford a 91% yield of propylene carbonate catalyzed by graphene oxide (GO) and tetrabutylammonium bromide (TBAB), avoiding conventional CO 2 compression and transportation. As expected, this study represents a potential large-scale application of integrating industrial solid waste management, carbon capture, and valorization to value-added chemicals and materials.
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Nature Communications
·
2026
·
IF 18.1
Ni Sulin,Xia Dong,Chen Can,Qiu Cheng,Li Youzhi,Yang Bin,Hou Yang,Lei Lecheng,Mao Zhengwei,Li Zhongjian
A hybrid system combining water electrolysis and H 2 autotrophic microorganism enables sustainable CO 2 valorization, but is hindered by low H 2 bioavailability and sluggish hydrogenase kinetics. Here, we report an interface-engineered inorganic–biological biohybrid, constructed by covalently anchoring iron single-atom catalysts (ISA) onto Cupriavidus necator ( C.N @ISA) via click chemistry. The ISA anchored interface generates a localized H 2 -rich microenvironment, accelerates H 2 dissociation, while the synergy between ISA and polyethylene glycol-phenylboronate linker stabilizes the inorganic-biological hybrid interface and promotes electron/proton transfer across microbial membrane. These coupled effects boost reduced form of nicotinamide adenine dinucleotide (NADH) regeneration and adenosine triphosphate (ATP) synthesis. In addition, ISA exhibits nanozyme-like activity, scavenging reactive oxygen species to protect cell viability. As a result, C.N @ISA achieves CO 2 -to-bioplastic poly- β -hydroxybutyrate production of 1058.8 mg L −1 with a Faradaic efficiency of 42.0%. Integrating theoretical calculations, electrochemical analysis, and transcriptomics confirms that ISA simultaneously enriches and activates H 2 while reinforcing intracellular metabolism, offering a generalizable strategy for carbon-negative biomanufacturing.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2026
·
IF 9.6
Weisong Feng,Manfen Liang,Yongjin Chen,Nuan Song,Lechen Diao,Zhichao Miao,Jin Zhou
Bismuth (Bi)-based catalysts are extensively employed for the electrocatalytic CO 2 reduction (ECR) for formate production. However, their practical application is constrained by inadequate catalytic activity and limited operational stability. In this study, two types of catalysts (carbon-supported Bi particles (Bi/C) and carbon-coated Bi particles (Bi@C)) were prepared via ligand modulation of Bi-based metal-organic frameworks. The role of interaction mode between Bi particles and carbon on the activity and stability was investigated. In contrast to the Bi/C catalyst, the coated carbon layer in the Bi@C catalyst improves charge transfer and optimizes the reaction kinetics, resulting in a higher current density and Faradaic efficiency of formate (FE formate ). Furthermore, the coated structure effectively stabilizes Bi active sites, thereby substantially improving activity in acidic electrolyte and long-term stability. The Bi@C catalyst exhibits remarkable stability in both alkaline (pH = 14.00) and acidic (pH = 1.00) electrolytes at 120 mA cm −2 , while preserving FE formate /FE HCOOH above 90%, showing promising potential for practical and industrial CO 2 electroreduction. This work can provide novel insights into the design of efficient and long-term stability Bi-based ECR catalysts.
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PubMed
高影响因子
Catalysts
·
2026
·Vol. 16
·期 4
·334
·
IF 4.5
Yu Chen,Xuan Chen,Huimei Wu,Hai-Jian Yang,Qingqing Jiang,Juncheng Hu,Cun-Yue Guo
The formylation of mercaptans using CO2as a C1 source represents a sustainable and efficient strategy for converting CO2into value-added chemicals. However, to date, S-formylation still remains scarcely explored with CO2as the starting material, despite its important role in various biological processes. In this work, the S-formylation reaction between CO2and mercaptans was successfully carried out to construct C-S bonds using an inexpensive and commercially available carboxylate salt (sodium edetate) as the catalyst under mild conditions (25 °C and 0.1 MPa). Further investigations demonstrated that the present catalytic system applies to a broad substrate scope, affording moderate to excellent yields in the S-formylation of both aliphatic and aromatic thiols with CO2. To clarify the excellent catalytic performance of carboxylates in these S-formylation reactions, reaction intermediates as well as the activating effects of carboxylates on carbon dioxide and phenylsilanes were identified through control experiments and spectroscopic analysis. Based on these findings, the reaction pathway of the S-formylation process was determined, and a corresponding reaction mechanism is proposed.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2026
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IF 3.9
Jianyang Wei,Lirong Wang,Guanhua Liu,Luting Wang,Liya Zhou,Yunting Liu,Xiaobing Zheng,Yanjun Jiang
The main challenges in electroenzymatic CO2 reduction are the low solubility of CO2 and the high cost of the cofactor. Inspired by eukaryotic cell structures, this study designed a hollow zeolite imidazole framework (H-ZIF-8) with the dual functions of capturing CO2 and immobilizing dual enzymes. This platform was coupled with electrochemical cofactor (reduced nicotinamide adenine dinucleotide, NADH) regeneration for enzymatic CO2 reduction. The hollow structure of ZIF-8 retained the activity of formate dehydrogenase (FDH) and carbonic anhydrase (CA) in the obtained FDH&CA@H-ZIF-8, while achieving efficient CO2 reduction using substrate enrichment by CA and ZIF-8. 2-Hydroxy-1,4-naphthoquinone (HNQ) served as an electron mediator in the electrocatalytic step. The electroenzymatic system produced 3.12 mM formate within 3 h, which was 7.3 times that of the free enzyme system. Meanwhile, the immobilized enzyme retained 80.1% of the initial enzyme activity after 8 reuse cycles with high storage stability. This strategy provided an effective platform for addressing the limitations of CO2 solubility and cofactor regeneration in enzymatic CO2 conversion.
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