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NATURE · 2024 ·Vol. 626 ·期 7997 ·86-91 · IF 50.5

Durable CO2 conversion in the proton-exchange membrane system

Fang Wensheng,Guo Wei,Lu Ruihu,Yan Ya,Liu Xiaokang,Wu Dan,Li Fu Min,Zhou Yansong,He Chaohui,Xia Chenfeng,Niu Huiting,Wang Sicong,Liu Youwen,Mao Yu,Zhang Chengyi,You Bo,Pang Yuanjie,Duan Lele,Yang Xuan,Song Fei,Zhai Tianyou,Wang Guoxiong,Guo Xingpeng,Tan Bien,Yao Tao,Wang Ziyun,Xia Bao Yu

Electrolysis that reduces carbon dioxide (CO 2 ) to useful chemicals can, in principle, contribute to a more sustainable and carbon-neutral future 1 , 2 , 3 , 4 , 5 , 6 . However, it remains challenging to develop this into a robust process because efficient conversion typically requires alkaline conditions in which CO 2 precipitates as carbonate, and this limits carbon utilization and the stability of the system 7 , 8 , 9 , 10 , 11 , 12 . Strategies such as physical washing, pulsed operation and the use of dipolar membranes can partially alleviate these problems but do not fully resolve them 11 , 13 , 14 , 15 . CO 2 electrolysis in acid electrolyte, where carbonate does not form, has therefore been explored as an ultimately more workable solution 16 , 17 , 18 . Herein we develop a proton-exchange membrane system that reduces CO 2 to formic acid at a catalyst that is derived from waste lead–acid batteries and in which a lattice carbon activation mechanism contributes. When coupling CO 2 reduction with hydrogen oxidation, formic acid is produced with over 93% Faradaic efficiency. The system is compatible with start-up/shut-down processes, achieves nearly 91% single-pass conversion efficiency for CO 2 at a current density of 600 mA cm −2 and cell voltage of 2.2 V and is shown to operate continuously for more than 5,200 h. We expect that this exceptional performance, enabled by the use of a robust and efficient catalyst, stable three-phase interface and durable membrane, will help advance the development of carbon-neutral technologies.

研究领域: 化学工程 · 能源科学 · 环境科学
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Fundamental Research · 2022 · IF 0

A recyclable method for titanium extraction and oxygen evolution from Ti−bearing slags

Zhenghao Pu,Wei Wang,Zhe Wang,Mingyin Kou,Yiwa Luo,Jianbang Ge,Xin Tao,Mingyong Wang,Shuqiang Jiao

Despite its existence for more than 80 years, the titanium industry is still challenged by massive carbon emissions, high production costs, and large resource waste. More than one hundred million tons of Ti−bearing blast furnace slag (TB−slag) has been discarded in China because of the difficulty of reutilization, which requires efficient titanium extraction and recovery technologies. This paper describes a low−cost, carbon−emission−free method for Ti extraction and oxygen evolution via molten oxide electrolysis (MOE) vacuum distillation. After a comprehensive analysis of the binding energies and activities of liquid metals, the highlights of our study are as follows. 1) Sb has the best preferential deposition of Ti among a series of high−Ti−affinitive liquid metal cathodes (Cu, Ni, Pb, Sn, and Sb). 2) The Ir anode was first used in TB−slag with IrO 2 formed on its surface to protect it from further corrosion. 3) An alloy containing Ti and Ca can be obtained by MOE, and Ti and Ca metals can be refined by further vacuum distillation. 4) A closed loop is formed in the overall process owing to the recyclable Sb cathode and continuous feeding of TB−slag into the electrolyte. This simple, low−cost, and environmentally friendly method can realize the efficient utilization of Ti resources and achieve carbon neutrality.

研究领域: 材料科学 · 环境工程 · 冶金工程
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Nano Energy · 2024 · IF 16.8

Self-adaptive energy-efficient windows with enhanced synergistic regulation of broadband infrared thermal radiation

Shangjing Li,Erqi Yang,Yiyi Li,Xiwei Mo,Zewen Chen,Zhengui Zhou,Guangming Tao,Yi Long,Bin Hu

Effective management of both near-infrared (NIR) radiation and long-wavelength infrared (LWIR) thermal emission through window design holds tremendous promise for achieving carbon neutrality in the building sector. Compared to the traditional static low emissivity (Low-E) and solar regulating windows, emerging emissivity-altering windows can better adapt to varied weather. However, dynamic windows with self-adaptive solar radiation and emissivity control have long been challenging, primarily due to the intricate broadband spectrum manipulation requiring sophisticated material design. Herein, by employing the NIR transparent hydrogen-doped In 2 O 3 (IHO) as a function layer ( ε = 0.13, T NIR = 79.8 %), we present a broadband self-adaptive radiative thermal management (SRTM) window based on Fabry-Perot resonator. Compared to the common tin-indium oxide (ITO)-based counterpart, the IHO-based SRTM window shows a 70 % enhancement in NIR power regulation ability (10.9 %) with remaining emissivity regulation ability (0.26). It contributes significantly to energy conservation offering an annual energy saving and equivalent CO 2 emissions reduction of up to 20 % (411 MJ·m −2 ) and 244 tons/yr, compared to traditional Low-E windows globally.

研究领域: 材料科学 · 建筑技术 · 能源工程
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Benefited wastewater utilization via configurable, spatialized, and microorganisms-integrated biophotonic systems

Yantong Liu,Longfei Chen,Le Yu,Jiaomeng Zhu,Fang Wang,Fenghua Jiang,Chengjun Sun,Li Zheng,Yi Yang

The development of engineering microbiology is widely expected to advance carbon neutrality and sustainability in the wastewater industry. Engineering microbiology can deliver desired functions without high treatment costs, complex processes, massive greenhouse gas emissions, and resource waste. Here, we propose a complementary strategy to realize benefited wastewater utilization by configurable spatialized microorganisms-integrated biophotonic systems (CSMBs). The configurable spatialized microorganisms enable enhanced microbial synergy and empower on-demand waste-to-bioenergy conversion through optofluidic-assisted design. The developed CSMBs improve the reaction between light and microorganisms (light harvesting and microorganisms’ photosynthesis) via enhanced natural light photon capture and adjustable optical wavelength. Thanks to these features, in prospective wastewater treatment, the CSMBs breakthrough achieve 89.89% and 91.8% degradation of total nitrogen (TN) and total phosphorus (TP) and 91.98% removal of chemical oxygen demand (COD) within 72 h, respectively. The biomass (the absorbance of 680 nm), lipid content, and chlorophyll-a content of Chlorella in the CSMBs were increased by 56.95%, 62.91%, and 35.41%, respectively, compared to the growth of single Chlorella . The method possesses broad applicability and superior tunability, which can be extended to a wide variety of wastewater treatment and enable more ability in benefited waste utilization.

CAS / MDL: 1338-43-8
研究领域: 环境科学 · 微生物学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

Co-precipitation synthesis of carbonic anhydrase-embedded magnetic zeolitic imidazolate framework-8 nanocomposite enzyme for enzymatic CO2 conversion and utilization in facilitating uranium extraction

Zhao Cui,Ting Li,Jing Sun,Qian Li,Hui Zhang,Guang-Yue Li

Carbonic anhydrase (CA)-mediated carbon conversion and utilization (CCU) technology is recognized as an eco-friendly and cost-effective strategy for carbon reduction. However, the broader application of this technology is significantly constrained by the operational instability and challenging recyclability of free CA . Fortunately, nano-integrated biocatalysis has emerged as an effective solution to these challenges. In this study, we immobilized CA for the first time as a CA-embedded ferriferous oxide-zeolite imidazolium framework-8 (Fe 3 O 4 @ZIF-8@CA) nanocomposite enzyme through a one-pot co-precipitation strategy, integrating both the in-situ growth of ZIF-8 around the Fe 3 O 4 core and the immobilization of CA within a single step. Subsequently, this nanocomposite was employed as a nano-integrated biocatalyst to facilitate an innovative CCU pathway. This pathway leverages bicarbonate, produced from the enzymatic hydration of carbon dioxide (CO 2 ), as a substantive uranyl complexing agent to facilitate the neutral leaching of sandstone uranium ore. Systematic characterization techniques, including SEM, TEM, XRD, FTIR, TGA, CLSM, and MPMS, confirmed that Fe 3 O 4 @ZIF-8@CA, which possesses a core–shell structure and excellent magnetic responsiveness, has been successfully synthesized. Enzymatic assays revealed that Fe 3 O 4 @ZIF-8@CA retains approximately 79% of the activity compared to its free counterparts while demonstrating significantly enhanced thermal and storage stability. The outcome of CO 2 hydration conversion for facilitating uranium extraction indicated that, compared with the non-enzymatic reaction group, the bicarbonate yield increased up to 1.5 times, and the uranium extraction efficiency was nearly 10% higher in the Fe 3 O 4 @ZIF-8@CA-mediated reaction group. These findings suggest that Fe 3 O 4 @ZIF-8@CA possesses excellent catalytic properties for CO 2 hydration and can achieve multiplied decarbonization by mediating this innovative CCU pathway. Furthermore, Fe 3 O 4 @ZIF-8@CA demonstrated superb reusability and durability, experiencing no significant degradation in its catalytic performance after eight consecutive hydration regeneration cycles. Our research is anticipated to be a viable option for advancing the goals of carbon neutrality and sustainable development.

研究领域: 生物催化 · 材料科学 · 环境科学
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Advanced Sustainable Systems · 2024 · IF 6.5

Solar Cells Manufactured Using Concentrated Solar Energy Toward Carbon Neutralization

Shuang Liu,Jiajia Huang,Liang Tu,Xiaohui Liu,Jing Zhang,Yuejin Zhu,Like Huang

The high photoelectric conversion efficiency (PCE) of solar cells and their environmentally friendly, low-carbon manufacturing processes are crucial for advancing carbon neutrality goals. This study introduces Fresnel lenses to focus sunlight for the sintering of mesoporous titanium dioxide (m-TiO 2 ) layers as an innovative method for fabricating perovskite solar cells (PSCs), effectively circumventing the energy-intensive and carbon-emitting high-temperature furnace sintering traditionally required. Through this concentrated solar annealing technique, an efficient and eco-friendly sintering of the m-TiO 2 layer is successfully achieved by removing organic residues from the precursor film and enhancing the film's transmittance, electrical conductivity, and grain size. Consequently, this has led to improved coverage of the perovskite layer and enhanced overall photovoltaic performance of the solar cells. Experimental results indicate that the m-TiO 2 film subjected to 60 min of concentrated sunlight sintering (CSS) demonstrates optimal photovoltaic performance, with the fabricated compact-layer-free PSCs achieving an impressive photoelectric conversion efficiency of up to 17.69%. This research not only offers a novel, cost-effective approach for the sustainable production of PSCs but also contributes tangible solutions for the green transformation of the photovoltaic industry and the achievement of carbon neutrality. This work points the way toward using solar energy to prepare solar power generation devices.

CAS / MDL: 67-68-5 68-12-2
研究领域: 材料科学 · 能源工程 · 环境科学
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Journal of CO2 Utilization · 2022 · IF 8.321

Construction of a gold-cobalt alloy catalyst to enhance the green reduction of carbon dioxide

Yuheng Zhou,Xiaohui Wang,Xubo Huang,Hui Deng,Yuntao Hu

Facilitating carbon neutrality to mitigate the greenhouse effect by an efficient means has great environmental and social value. In this research, the Au-Co catalyst is synthesized with a developed non-aqueous solvent strategy. By tuning the ratio of the bimetallic composition, it represents a prominent catalytic activity in the reduction of CO 2 with benzyl alcohol as the hydrogen donor. By means of the anaerobic oxidation of benzyl alcohol, CO 2 can be reduced to methanol as well as methyl benzoate as the main product with a high turnover frequency (1079 h −1 ) at 220 °C. Taking advantage of a series of characterizations and DFT calculation , it is revealed that the catalytic system constructed in this research promotes the adsorption and activation of CO 2 . These results demonstrate a feasible route to develop hydrogen-free utilization of CO 2 to achieve environmental carbon neutrality in the future.

CAS / MDL: 78-10-4 67-66-3
研究领域: 环境科学 · 材料科学 · 化学工程
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Small · 2023 ·Vol. 19 ·期 33 ·2301498 · IF 13.3

High-Performance Li-CO2 Battery Based on Carbon-Free Porous Ru@QNFs Cathode

Ting Zhu,Sheng Wang,Zhiqian Yu,Hucheng Song,Jun Xu,Kunji Chen

Lithium-carbon dioxide (Li-CO 2 ) batteries have attracted much attention due to their high theoretical energy density. However, due to the existance of lithium carbonate and amorphous carbon in the discharge products that are difficult to decompose, the battery shows low coulombic efficiency and poor cycle performance. Here, by adjusting the adsorption of carbon dioxide (CO 2 ) on ruthenium (Ru) catalysts surface, this work reports an ultralow charge overpotential and long cycle life Li-CO 2 battery that consists of typical lithium metal, ternary molten salt electrolyte (TMSE), and Ru-based cathode. Experimental results show that the Ru catalysts deposited on quartz nanofiber (QF) can suppress the four-electron conversion of CO 2 to lithium carbonate (Li 2 CO 3 ). As a result, the battery shows a long-cycle-life of over 457 cycles at 1.0 A g −1 with a limited capacity of 500 mAh g −1 Ru . Remarkably, a recorded low discharge potential of ≈3.0 V has been achieved after 35 cycles at 0.5 A g −1 , with a charge potential retention of over 99%. Moreover, the battery can operate over 25 A g −1 and recover 96% potential. This battery technology paves the way for designing high-performance rechargeable Li-CO 2 batteries with carbon neutrality.

研究领域: 材料科学 · 电化学
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CHEMICAL ENGINEERING SCIENCE · 2024 · IF 4.1

Boosting catalytic activity of Ni/ZrO2 by introducing MoO3 on selective hydrogenolysis of lignin

Fenghao Shu,Guangcai Long,Yanwu Chen,Ying Gao,Menghao Jiang,Jinxing Long

Conversion of renewable lignin to value-added aromatic chemicals presents a broad prospect to achieve the goals of “carbon neutrality”. In this work, an efficient approach is proposed for selective hydrogenolysis of lignin to valuable 4-propyl syringol in the presence of cost-effective catalyst of y Ni/ZrO 2 - x MoO 3 . When the lignin hydrogenolysis is performed with 15Ni/ZrO 2 -10MoO 3 , 15.4% yield of monophenols is achieved, which is approximately twice as that from the 15Ni/ZrO 2 catalytic system (7.8%). Importantly, 33.1% of these monophenols are identified as 4-propyl syringol (4-PS), a versatile fine chemical. An extensive characterization of the modified catalysts by means of XRD, nitrogen adsorption–desorption isotherm, SEM, TEM, XPS, NH 3 -TPD, CO 2 -TPD, and H 2 -TPR, confirms that the introduction of MoO 3 changes the primary phase of ZrO 2 and the acidity/basicity properties of catalyst. As a result, an enhanced cleavage of the C-O linkage between S-lignin and other units is demonstrated, which consequently contributes to the good selectivity of 4-propyl syringol. Therefore, this work provides a new insight for producing bulk aromatic chemicals via a sustainable route.

研究领域: 化学工程 · 可再生资源利用
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2024 · IF 7.7

Robust fluorinated cellulose composite aerogels incorporating radiative cooling and thermal insulation for regionally adaptable building thermal management

Yanmei Liu,Xiaohai Bu,Runqi Liu,Minxing Feng,Zewu Zhang,Zhou Yuming

Passive radiative cooling (PRC) is an emerging sustainable technology that plays a key role for achieving the goal of carbon neutrality. However, several challenges remain for PRC materials in their practical application in building thermal management, including overcooling problems and unsatisfactory cooling efficiency caused by solar absorption and parasitic heat gains. In this work, fluorinated cellulose-based composite aerogels (FCCA) integrating thermal insulation and PRC were developed by a facile manufacturing strategy that combined phase separation and freeze-drying. P(VdF-HFP) was utilized to promote the formation of nano/micro porous architectures in FCCA, resulting in a decrease in the thermal conductivity of the aerogel to 0.034 W m −1  K −1 while simultaneously increasing its solar reflectance and infrared emissivity (8–13 μm) to 95.74 % and 97.15 %, respectively. The aerogel cooler achieved a sub-ambient cooling temperature of ∼9.68 °C during the daytime and maintained its cooling effectiveness even on cloudy days. The fluorinated aerogels demonstrated excellent hydrophobicity and chemical durability after outdoor exposure and heat aging tests. This work opens up a new pathway to design low-cost cellulose-based materials for efficient thermal management of energy-saving buildings around the world.

研究领域: 材料科学 · 可持续能源 · 建筑工程
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CERAMICS INTERNATIONAL · 2024 · IF 5.1

In-situ growth of Cs0·33WO3@ATO composite material with enhanced NIR shielding rate for energy-saving coating

Qingguo Cai,Xin Li,Liying Wen,Yangfan Du,Yihan Shi,Yibo Sun,Bo Ding,Yuanhao Wang,Shifeng Wang

Driven by the global goal of “carbon neutrality”, energy conservation, emission reduction and low-carbon development have become important research directions. Transparent thermal insulation materials can effectively shield near-infrared radiation while maintaining high visible light transmittance , making them widely applicable in building energy conservation . In this paper, antimony-doped tin oxide (ATO) and cesium tungsten bronze (Cs x WO 3 , or CWO) are chosen to be composited in order to solve the problems of the poor shielding effect of ATO for short-wavelength near-infrared (NIR) light and the unsatisfactory shielding effect of CWO for long-wavelength NIR light. Therefore, in this study, we employed a one-step hydrothermal method to form a novel CWO@ATO core-shell structure to combine the advantages of both ATO and CWO. By adjusting the composite ratio of ATO and CWO, both the physical and electronic stucutres are effectively tuned to promote the optical modulation in a broad bandwidth. Enventually, the core-shell structured composite exhibit an excellent near-infrared blocking property, surpassing the pure ATO by 27.8 % in the wavelength region of 780∼1500 nm while improving by 14.9 % compared to CWO in the long wavelength between 1500 and 2500 nm. Furthermore, the prepared CWO@ATO core-shell structure repesents near-infrared shielding rate as high as 93.1 % in the full NIR spectrum , and possesses an overall thermal insulation coefficiency (THI) of 9.33 in the full range from 780 nm to 2500 nm, which is substantially larger than that of pure ATO and CWO by a factor of 2.37 and 3.05, respectively. This core-shell structure engineering realizes the utilization of complementary advantages of ATO and Cs 0·33 WO 3 materials, providing a new method to improve the near-infrared performance of energy-saving glass coating , and having broad application prospects in the field of low-carbon buildings.

研究领域: 材料科学 · 能源科学
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CATALYSIS LETTERS · 2022 ·Vol. 153 ·期 1 ·271-284 · IF 2.936

Dual Nature Cupper-Based Ionic Liquid-Assisted n-Butane Selective Oxidation with a Vanadium Phosphorus Oxide Catalyst

Faizan Muhammad,Zhang Ruirui,Liu Ruixia

Recently, global warming is proving to be an increasing challenge for the sustainable human survival on planet earth. Worldwide, researchers are putting their efforts into controlling carbon emissions and have set the aim to achieve levels of overall carbon neutrality. Different industrial processes, especially oil refinery processes, release large amounts of low-carbon alkanes as gaseous byproducts directly into the air and pollute clean environments, which is one of the major reasons for sudden climate changes, ocean acidification, loss of biodiversity, and rising sea levels. The conversion of lighter alkanes, especially n-butane, into value-added chemicals can be beneficial for green economies and green environments. Presently, heterogeneous vanadium phosphorus oxide catalysts (VPOs) are considered potential candidates for n-butane selective oxidation toward maleic anhydride (MA). In this research, we developed a VPO catalyst with the assistance of copper-based ionic liquids (Cu-ILs), including [Bmim][OAc]–[Cu(OAc) 2 ], [Bmim][Cl]–[CuCl], and [Bmim][Cl]–[CuCl 2 ]. We observed significant improvement in the MA selectivity; meanwhile, the CO x (CO and CO 2 ) selectivity was decreased. Compared to the unpromoted catalyst (Blank-VPO), the Cu-IL-promoted catalyst, i.e., [Bmim][Cl]–[CuCl 2 ]-VPO remarkably increased the MA selectivity (11%) and n-butane conversion (9.2%) and minimized the CO x selectivity (11%). In addition to this the ratio of CO/CO 2 has been reduced from 2.01 to 1.32. Therefore, this can be a helpful process for achieving carbon neutrality goals. Graphical Abstract

研究领域: 化学工程 · 环境科学 · 催化化学
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