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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

A novel membrane-promoted crystallization process integrating water recovery and salt production for brine management

Guozhao Ji,Weijian Wang,Huihuang Chen,Siyuan Yang,Jing Sun,Weng Fu,Zhiqiang Huang,Bo Yang

Brine management is one of the global challenges nowadays. Herein, by taking advantage of capillary forces and low-grade heat (50 °C), we propose a novel ceramic membrane-promoted crystallization (MPC) process for brine management. The MPC process simplifies the traditional multiple energy-intensive steps and dispenses the use of expensive anticorrosive equipment via adopting three hierarchical layers (α-Al 2 O 3 substrate, γ-Al 2 O 3 interlayer, and SiO 2 top layer). The hydrophilic mesoporous SiO 2 top layer provides continuous driving force for brine solution transport from the inner shell of the membrane toward the outer surface, where heterogenous nucleation and secondary nucleation occur to form numerous long needle-like salt whiskers. The growth kinetics of salt whiskers accelerates with time as the formed salt whiskers provide extra evaporation area to intensify water evaporation. Template-directing molecules P123 significantly enhance the specific surface area, pore volume, pore size, and pore regularity of the SiO 2 top layer, thereby promoting both water recovery and salt production. The optimized membrane displays high water recovery (790.3 g m −2 ) and salt production (194.6 g m −2 ) for high-salinity brine (20 wt%). Moreover, the MPC process demonstrates high performance, mechanical stability and thermal durability during the long-term test. It is expected that the MPC process would provide an innovative zero-liquid discharge approach for the efficient and low-cost brine management.

研究领域: 环境科学 · 材料科学
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Science China-Chemistry · 2025 · IF 9.7

Dual roles of the sacrificial agent in efficient solar-to-chemical production by nonphotosynthetic Moorella thermoacetica

Bai Rui,Li Junpeng,Chen Wei,He Yi,Zhou Xudong,Tian Xiaochun,Ren Chongyuan,Chen Liqi,Xiao Yong,Zhao Feng

The integration of microorganisms and photosensitizers presents a promising approach to chemical production utilizing solar energy. However, the current system construction process remains complex. Herein, we introduce a straightforward and efficient solar-to-chemical conversion system that combines the dissolved photosensitizer Eosin Y with the non-photosynthetic bacterium Moorella thermoacetica . Under light radiation, acetate production increased to 5.1 µM h −1 µM −1 catalyst, exceeding the previously reported maximum by 5.9-fold, with a quantum efficiency of 17.6%. The soluble photosensitizer EY can penetrate the cell and directly engage in intracellular energy metabolism, significantly enhancing intracellular ATP and NADPH/NADP + levels. Within this biohybrid system, sacrificial agent triethanolamine played a dual role: (1) providing continuous photoelectron generation by Eosin Y, enhancing intracellular reducing power, and facilitating carbon fixation via the Wood-Ljungdahl pathway; and (2) its oxidation product, formaldehyde, served as a critical intermediate and a direct precursor for methylenete-trahydrofolate in the Wood-Ljungdahl pathway, consequently simplifying reaction steps and markedly boosting acetate yield. This study provides a simple microorganism-photosensitizer biohybrid system to produce acetate and light on the multifaceted roles of sacrificial agents, paving the development of efficient solar energy conversion with nonphotosynthetic bacteria.

研究领域: 微生物学 · 生物能源 · 合成生物学
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mSphere · 2024 · IF 3.7

Anaerostipes hadrus, a butyrate-producing bacterium capable of metabolizing 5-fluorouracil

Danping Liu,Li-Sheng Xie,Shitao Lian,Kexin Li,Yun Yang,Wen-Zhao Wang,Songnian Hu,Shuang-Jiang Liu,Chang Liu,Zilong He

Anaerostipes hadrus (A. hadrus) is a dominant species in the human gut microbiota and considered a beneficial bacterium for producing probiotic butyrate. However, recent studies have suggested that A. hadrus may negatively affect the host through synthesizing fatty acid and metabolizing the anticancer drug 5-fluorouracil, indicating that the impact of A. hadrus is complex and unclear. Therefore, comprehensive genomic studies on A. hadrus need to be performed. We integrated 527 high-quality public A. hadrus genomes and five distinct metagenomic cohorts. We analyzed these data using the approaches of comparative genomics, metagenomics, and protein structure prediction. We also performed validations with culture-based in vitro assays. We constructed the first large-scale pan-genome of A. hadrus (n = 527) and identified 5-fluorouracil metabolism genes as ubiquitous in A. hadrus genomes as butyrate-producing genes. Metagenomic analysis revealed the wide and stable distribution of A. hadrus in healthy individuals, patients with inflammatory bowel disease, and patients with colorectal cancer, with healthy individuals carrying more A. hadrus. The predicted high-quality protein structure indicated that A. hadrus might metabolize 5-fluorouracil by producing bacterial dihydropyrimidine dehydrogenase (encoded by the preTA operon). Through in vitro assays, we validated the short-chain fatty acid production and 5-fluorouracil metabolism abilities of A. hadrus. We observed for the first time that A. hadrus can convert 5-fluorouracil to α-fluoro-β-ureidopropionic acid, which may result from the combined action of the preTA operon and adjacent hydA (encoding bacterial dihydropyrimidinase). Our results offer novel understandings of A. hadrus, exceptionally functional features, and potential applications.

CAS / MDL: 51-21-8
研究领域: 微生物学 · 基因组学 · 医学
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2024 · IF 20.2

Dynamic Fe-O-Cu induced electronic structure modulation on CuOx electrode for selective electrocatalytic oxidation of glycerol

Sheng Zhong,Bin He,Shuang Wei,Ruirui Wang,Ruirui Zhang,Ruixia Liu

Electrocatalytic glycerol oxidation reaction to produce high-value organic chemicals has research significance for managing the overproduction of glycerol and handling the energy crisis. Herein, a copper-based self-supporting catalytic electrode with a dynamic Fe-O-Cu optimized coordination (Fe-CuO x /CF) was prepared. The oxygen-bridged asymmetric coordination structure (Fe-O-Cu) optimized the electronic configuration and promoted the formation of the crucial intermediate species. After Fe was embedded in the lattice of copper oxides, a remarkable enhancement in the adsorption capacity of OH - and glycerol was confirmed. As a result, Fe-CuO x /CF exhibited an excellent production capacity of formate, with high faradaic efficiency and selectivity values of 93.65 % and 95.10 %. Concurrent production of formate and high purity hydrogen was achieved in the double-electrode flow electrolyzer. This work provides guiding significance for the optimization of the catalytic coordination and the design of high-efficiency transition metal-based catalysts for electrooxidation of biomass platform molecules.

研究领域: 电化学 · 催化材料 · 能源化学
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ACS Sustainable Chemistry & Engineering · 2024 · IF 7.1

Boosting Microbial CO2 Electroreduction by the Biocompatible and Electroactive Bimetallic Fe–Mn Oxide Cathode for Acetate Production

Jin Du,Hebin Liang,Yubin Zou,Bing Li,Xiao-yan Li,Lin Lin

The electroreduction of carbon dioxide (CO2) to high-value organic chemicals by the microbial electrosynthesis (MES) system relies heavily on the electrochemical properties of the electrode materials. In this work, CO2 reduction for acetate production was greatly boosted by decorating the carbon felt cathode using the Fe–Mn bimetallic oxides, using an enriched anaerobic mixed culture dominated by the homoacetogen Acetobacterium wieringae. In comparison with the unmodified carbon felt as the cathode in the MES reactor, modification with MnFe2O4 increased the acetate production rate from 28 to 78 g/(m2·d), higher than those with MnO at 59 g/(m2·d) and Fe2O3 at 62 g/(m2·d), and the relative abundance of A. wieringae increased dramatically from 51 to 87% in the biofilm. This was probably due to the mediated electron uptake via the redox cycles of Mn(III)/(II) and Fe(III)/(II), improved specific surface area, and enhanced hydrophilicity of the cathode, benefiting from the synergistic effect of Fe and Mn ions. Overall, this study provides a facile and promising electrode modification strategy for MES with Fe–Mn bimetallic oxides for efficient CO2 conversion and acetate production, bringing the world closer to achieving carbon neutrality.

CAS / MDL: 1309-37-1 1344-43-0
研究领域: 环境科学 · 生物技术 · 电化学 · 微生物学
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2025 · IF 21.1

Boosting seawater desalination driven by electroreduction of CO2 to formate on bimetallic Sn/Cu polyphthalocyanine frameworks

Minzhang Li,Man Liang,Wei Wang,Beichi Luo,Yanhong Ji,Longzhang Dong,Lu Guo,Danling Tang,Guangguo Ying,Fuming Chen

Electrochemical desalination offers a promising route to address water scarcity, but current methods often face limitations in salt removal rate and capacity. This study introduces an ultrafast electrocatalytic desalination system that leverages the electrochemical reduction of CO 2 to formate (CO 2 RR) to drive efficient salt removal. The optimized bimetallic Sn/Cu-based polyphthalocyanine (Sn 2 Cu 1 PPc) exhibits exceptional CO 2 RR performance, achieving a peak FE formate of 90.3 % at −1.0 V vs. RHE and a j formate of 84.8 mA cm −2 . In-situ spectroscopic analysis and density functional theory (DFT) calculations reveal that the incorporation of Cu-N 4 units into the Sn-based polyphthalocyanine (SnPPc) promotes CO 2 adsorption and facilitates active hydrogen provision, leading to the observed enhancement in CO 2 RR activity. Using the Sn 2 Cu 1 PPc catalyst, our system achieves a salt removal rate of 1701.3 μg cm −2 min −1 and a formate production rate of 0.79 mmol h −1 cm −2 when treating natural seawater, resulting in potable water with 99.06 % salt removal efficiency. This performance is enabled by a high current density (∼70 mA cm −2 ) during CO 2 RR, which significantly enhances ion transport across the membranes, making this one of the most effective desalination approaches reported. This work demonstrates the potential of coupling CO 2 RR with desalination for sustainable water production and CO 2 mitigation, while also advancing the design of efficient Sn-based electrocatalysts for formate production.

研究领域: 电化学 · 环境科学 · 材料科学 · 能量转换 · 水处理
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JOURNAL OF ALLOYS AND COMPOUNDS · 2025 · IF 6.3

Construction of a bifunctional SnCo alloy electrode by one-step electrodeposition for electrocatalytic simultaneous production of formate from CO2 and glucose

Chongyan Chen,Shuguang Shen,Jie Wang,Xingting Guo,Lili Zhang,Yongmei Liu,Jing Li

Replacing the oxygen evolution reaction (OER) with small molecule oxidation coupled with CO 2 reduction reaction (CO 2 RR) has become an effective strategy to reduce the energy demand of electrolyzers. However, the inconsistency of the cathode and anode products caused additional separation costs. Therefore, the selection of anodic paired-reactions capable of directing the same product is a key measure to solve the problem. At the same time, this poses a challenge for the design of bifunctional electrodes suitable for redox coupling systems. Herein, we established a coupled system in which the glucose oxidation reaction (GOR) is paired with the formate production via CO 2 RR, and for the first time, we have calculated its advantages through thermodynamic analysis. Additionally, a Sn 76.8 Co 23.2 electrode featuring crystalline Sn/amorphous SnCo heterointerfaces was prepared utilizing a revolutionary one-step in-situ electrodeposition method. It was demonstrated that the abundant two-phase interfaces optimized the redistribution of electrons, and that electrons transfer from Sn atoms to Co atoms to favor the adsorption of oxygen-containing intermediates, thereby improving the catalytic capability of Sn 76.8 Co 23.2 in the CO 2 RR, GOR semi-reaction, and CO 2 RR//GOR coupled system. This work provides invaluable insights into the matching of reactants and products for co-electrolysis systems, as well as a meaningful idea for the design of bifunctional electrocatalysts.

CAS / MDL: 12058-66-1 7646-79-9
研究领域: 电化学 · 材料科学 · 催化 · 能量转换 · 环境工程
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ACS Sustainable Chemistry & Engineering · 2024 · IF 7.1

Implanting CuNi Alloy into NiVOx for H2 Evolution with Ultralow Overpotential and Highly Selective Formate Production

Ying Wu,Wenhui Fang,Min Li,Yutao Cao,Wei Cui,Zengxi Li,Hong Zhao

Electrochemical upgrading of biomass waste (such as glycerol)-assisted water electrolysis for the production of valuable formate and high-purity hydrogen offers a promising route to develop sustainable and clean sources of energy. Herein, using a simple two-step electrodeposition method to implant CuNi alloy in VOx-doped Ni (NiVOx), we construct a competent, stable, and bifunctional heterogeneous catalyst (CuNi–NiVOx) toward hydrogen evolution reaction (HER) and glycerol electrooxidation reaction (GER). The CuNi–NiVOx electrode presents excellent HER activity with an ultralow overpotential of 8 mV in 1.0 M KOH to deliver a current density of 10 mA cm–2 and high GER activity for selective formate production with high Faradaic efficiency (FE). Moreover, the hybrid electrolytic cell formed by the bifunctional CuNi–NiVOx catalyst was able to reach a current density of 10 mA cm–2 with an ultralow voltage (1.308 V). X-ray photoelectron spectroscopy (XPS) and density functional theory (DFT) calculations confirm the existence of electron transfer between the O sites and metal sites and between heterogeneous interfaces, thus optimizing the hydrogen adsorption ability (0.02 eV). This work may provide ideas for the engineering of heterogeneous dual-function electrocatalysts for energy-saving hydrogen production and simultaneous highly selective production of formate.

研究领域: 电化学 · 催化 · 能源材料 · 可再生能源
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2021 · IF 19.503

In-Sn alloy core-shell nanoparticles: In-doped SnOx shell enables high stability and activity towards selective formate production from electrochemical reduction of CO2

Jigang Wang,Shunlian Ning,Mi Luo,Dong Xiang,Wei Chen,Xiongwu Kang,Zheng Jiang,Shaowei Chen

SnO 2 has been recognized as excellent catalyst towards formate production from electrochemical CO 2 reduction (CO 2 R). However, it is a great challenge to prepare SnO 2 that is stable under the working condition of CO 2 R and the active center of the SnO 2 -based catalyst towards CO 2 R has been illusive. In this work, Sn-In alloy nanoparticles display an InSn 4 intermetallic core and an amorphous In-doped tin oxide shell and a CO 2 -to-formate faradaic efficiency of 94% and a current density of 236 mA cm −2 was achieved at −0.98 V. Operando X-ray absorption and Raman spectroscopy reveal that the In-doped tin oxide shell remains stable under CO 2 R condition. Density functional theory calculations indicate that the In-doped tin oxide results in the formation of oxygen vacancy, stabilized tin oxide shell and exergonic pathway for CO 2 -to-formate, which might account for the high performance of the catalysts towards CO 2 R.

研究领域: 材料科学 · 电化学 · 催化 · 可持续能源
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ACS Nano · 2025 · IF 16

Integration of Nitrate Denitrification and Biomass Valorization in a Water-Splitting-Based Configuration for Concurrent Electrocatalytic Refining

Yuchan Li,Baojun Long,Yanjia Cui,Wenqing Li,Dong He,Zunjian Ke,Xiangheng Xiao

Engineering anodic and cathodic half-reactions with more favorable thermodynamics and techno-economics in water-splitting cells for electrorefining offers a promising approach to producing green fuels and fine chemicals. Herein, we demonstrated a coelectrolysis system integrating nitrate reduction reaction (NO3RR) and biomass oxidation reaction (BOR), where a well-designed CuNi alloy acted as the catalyst at the cathode and anode. The CuNi delivered a yield rate of 2.87 mmol h–1 cm–2 (8.44 mmol h–1 mgcat–1) at 0 V vs RHE and a FE of 95.33% (a current density of −136 mA cm–2) at −0.2 V vs RHE for ammonia synthesis from nitrate reduction. Mechanistic studies revealed that Cu centers rapidly converted NO3– to NO2–, while Ni sites promoted water dissociation, generating *H species for intermediate deoxygenation and hydrogenation via stepwise proton transfer. At the anode, the CuNi efficiently catalyzed the oxidative upgradation of biomass derivatives, with a Faradaic efficiency of >90% and a long-term stability over 240 h for formate production. In situ experiments demonstrate that Cu substantially enhances the dynamic transformation efficiency of the NiIII–O active species on CuNi catalysts. The integrated NO3RR||BOR system demonstrated an efficient and stable electrosynthesis (>120 h) of ammonia (∼3.9 mmol h–1 cm–2 or 11.47 mmol h–1 mgcat–1) and formate (∼38.3 mmol h–1 cm–2 or 112.65 mmol h–1 mgcat–1). This study emphasizes the design of a hybrid system for electrocatalytic refining of waste feedstocks into commodity chemicals.

研究领域: 电化学 · 催化 · 环境工程 · 能量转换 · 绿色化学 · 材料科学 · 可持续化学
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Materials Chemistry Frontiers · 2023 ·Vol. 7 ·期 16 ·3382-3389 · IF 7

Structural reconstruction of BiPbO2Br nanosheets for electrochemical CO2 reduction to formate

Gaoming Sun,Chong Zou,Wen Sun,Ying Fang,Shuijian He,Yana Liu,Jiguang Zhang,Yunfeng Zhu,Jun Wang

The electrochemical reduction of CO2 to value-added products represents a promising strategy to store renewable energy and realize global carbon neutrality. Bi-based materials have attracted extensive attention for formate production from CO2 reduction. Herein, we employ BiPbO2Br nanosheets as the bimetallic oxyhalide precursor to prepare a reconstructed Bi–Pb composite catalyst by electroreduction. The resultant catalyst exhibits impressive performance for formate production, including a high partial current density (40 mA cm−2 at −1.0 V), a high faradaic efficiency (96.6% at −0.9 V), a high energy conversion efficiency (>50% from −0.8 to −1.1 V), and good stability. As compared with the monometallic Bi and Pb counterparts, the Bi–Pb composite catalyst demonstrates superior intrinsic performance, which is attributed to the multiphase composites and abundant heterogeneous interfaces derived from electroreduction induced structural reconstruction of BiPbO2Br. This work offers an attractive strategy to further improve the performance of Bi catalysts for CO2 reduction to formate.

研究领域: 电化学 · 材料科学 · 催化 · 能源存储 · 环境科学
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Nature Communications · 2022 ·Vol. 13 ·期 1 ·1-16 · IF 17.694

Functional and metabolic alterations of gut microbiota in children with new-onset type 1 diabetes

Yuan Xiaoxiao,Wang Ruirui,Han Bing,Sun ChengJun,Chen Ruimin,Wei Haiyan,Chen Linqi,Du Hongwei,Li Guimei,Yang Yu,Chen Xiaojuan,Cui Lanwei,Xu Zhenran,Fu Junfen,Wu Jin,Gu Wei,Chen Zhihong,Fang Xin,Yang Hongxiu,Su Zhe,Wu Jing,Li Qiuyue,Zhang Miaoying,Zhou Yufeng,Zhang Lei,Ji Guang,Luo Feihong

Gut dysbiosis has been linked to type 1 diabetes (T1D); however, microbial capacity in T1D remains unclear. Here, we integratively profiled gut microbial functional and metabolic alterations in children with new-onset T1D in independent cohorts and investigated the underlying mechanisms. In T1D, the microbiota was characterized by decreased butyrate production and bile acid metabolism and increased lipopolysaccharide biosynthesis at the species, gene, and metabolite levels. The combination of 18 bacterial species and fecal metabolites provided excellently discriminatory power for T1D. Gut microbiota from children with T1D induced elevated fasting glucose levels and declined insulin sensitivity in antibiotic-treated mice. In streptozotocin-induced T1D mice, butyrate and lipopolysaccharide exerted protective and destructive effects on islet structure and function, respectively. Lipopolysaccharide aggravated the pancreatic inflammatory response, while butyrate activated Insulin1 and Insulin2 gene expression. Our study revealed perturbed microbial functional and metabolic traits in T1D, providing potential avenues for microbiome-based prevention and intervention for T1D.

研究领域: 微生物学 · 内分泌学 · 代谢组学 · 免疫学
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