Nature Communications
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2025
·Vol. 16
·期 1
·1-12
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IF 15.7
Xu Feiyan,Zhao Feifan,Deng Xianyu,Zhang Jinfeng,Zhang Jianjun,Ai Chenbin,Yu Jiaguo,García Hermenegildo
The rapid increase in atmospheric CO 2 levels due to industrialization underscores the urgent need for innovative carbon valorization strategies. Photocatalytic CO 2 reduction presents a sustainable solution; however, conventional systems suffer from inefficient charge separation and limited product applicability. Herein, a green and scalable tandem strategy is developed by integrating S-scheme photocatalysis with palladium-catalyzed carbonylation. A rationally designed CeO 2 /Bi 2 S 3 heterojunction leverages its hierarchical structure, broad visible-light absorption, oxygen-vacancy-mediated charge dynamics, and the S-scheme charge transfer mechanism to achieve highly efficient photocatalytic CO 2 -to-CO conversion (14.05 mmol g −1 , 98% selectivity). The generated CO is directly utilized in a subsequent carbonylation reaction under mild conditions, yielding high-value amides with near-quantitative CO utilization. This integrated approach eliminates the risks of CO handling and enhances economic viability, providing a direct and effective route for converting CO 2 into fine chemicals. By bridging photocatalysis with industrial catalysis, this work advances sustainable carbon recycling technologies and opens avenues for the development of efficient CO 2 conversion systems.
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Nano Materials Science
·
2025
·
IF 17.9
Yang He,Qingling Ruan,Han Kang,Ling Ye,Ya-Xiong Wang,Tiefeng Liu,Hairong Cheng,Xingxing Gu
Li-S batteries (LSBs), with their exceptional theoretical energy density, are widely recognized as a leading option for future energy storage solutions. Nevertheless, on the way to commercialization, the poor conductivity of the positive electrode, the easy dissolution loss of the active substance, and the serious dendrite growth of the negative electrode are stumbling blocks. Therefore, this work designs a novel tungsten and nitrogen-co-doped nanoporous carbon (W,N-C) with multifunction: chemically adsorbs the polysulfides to inhibit shuttling behavior, accelerates Li + transfer, and catalyzes polysulfides redox to address the aforementioned issues of LSBs. As expected at the beginning of the design, the prepared W,N-C-5/S composites cathodes demonstrate excellent performances, i.e., delivering an initial capacity of 944.9 mAh g −1 and a reversible capacity of 771.7 mAh g −1 after 500 cycles at 1 C, significantly outperforming the N-C/S contrast sample. The proposed method offers a feasible solution for boosting the electrochemical performance of LSBs.
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INORGANIC CHEMISTRY COMMUNICATIONS
·
2024
·
IF 4.4
Huadong Liu,Hao Sun,XiaoYu Sun,Jing liang Cheng
This paper presents a novel tubular microreactor immobilized a photocatalyst to overcome the limitations of low light utilization and the challenges associated with catalyst recovery in traditional photocatalysis reactors. The copper-sulfur co-doped carbon quantum dots (Cu, S-CQDs)/bismuth vanadate (BiVO 4 ) composites were successfully immobilized on the inner surface of the microreactor channel through the sol–gel process. The catalytic layer in the microreactor enlarged the specific surface area and facilitated the mass transfer. Meanwhile, it also greatly reduced the consumption of chemical supplies and eliminated the need for recycling the photocatalyst. The morphology and structural features of the catalytic layer were studied by characterization. Then the photocatalytic performance of the microreactor was evaluated by photocatalytic degradation of Rhodamine B. The photocatalytic kinetics of the photocatalytic reaction in the microreactor was 0.60925, which was 10.49 times greater than that in the macroscopic system. The results showed that the microreactor led to a significant improvement in degradation efficiency. The reproducibility experiments conducted on the microreactor system further demonstrate its excellent stability. In short, integrating the beneficial properties of microreactors with Cu, S-CQDs/BiVO 4 exhibits highly promising prospects of photocatalytic applications.
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CHINESE JOURNAL OF CATALYSIS
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2025
·
IF 17.7
Xinyue Tan,Minghui Zhang,Yang Bai,Xiaoyu Liu,Jianfang Jing,Yiguo Su
The major challenge in photocatalytic water splitting lies in water oxidation reactions, which still suffer from poor charge separation. This study overcame inefficient charge separation by establishing a robust interfacial electric field through the electrostatic-driven assembly of Co 3 O 4 nanoparticles with a perylene imide supramolecule (PDINH). The well-aligned band structures and intimate interfacial contact in the PDINH/Co 3 O 4 heterostructure create an enhanced interfacial electric field that is 4.1- and 53.2-fold stronger than those of individual PDINH and Co 3 O 4 , thus promoting directional charge separation and transfer. Moreover, S-scheme charge transfer strongly preserves the oxidative holes in PDINH to drive efficient water oxidation reactions. Consequently, PDINH/Co 3 O 4 composite achieves a photocatalytic oxygen evolution rate of 29.26 mmol g –1 h –1 under visible light irradiation, 8.2-fold improvement over pristine PDINH, with an apparent quantum yield of 6.66% at 420 nm. This study provides fundamental insights into interfacial electric field control for the development of high-performance organic photocatalysts for efficient water oxidation.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
·
IF 9.4
Haidong Luo,Shengjiang Zhang,Fozia Batool,Suhang Chen,Fengqi Zhao,Kangzhen Xu
The construction of an S-scheme heterostructure is considered as a promising strategy for enhancing photocatalytic performance. Herein, a three-dimensional Bi 5 O 7 I (BOI) microsphere decorated with Bi 2 Sn 2 O 7 (BSO) nanoparticles was prepared for the first time via a simple ultrasonic-assisted electrostatic self-assembly strategy and used for the degradation of 2,4-dinitrophenylhydrazine. 3 wt% Bi 2 Sn 2 O 7 /Bi 5 O 7 I has the highest degradation activity (93.7 %), with an apparent rate constant of 0.0848 min −1 , which is 2.55 times that of the original Bi 5 O 7 I (0.0333 min −1 ). Moreover, the optimal binary heterojunction photocatalyst has good reusability and universal applicability. The results of cyclic voltammetry tests clarify that the optimal photocatalyst can provide more surface reactive sites. The results of radical trapping experiments and electron spin resonance indicate that holes (h + ) and superoxide radicals are the main active radicals in the degradation process of 2,4-dinitrophenylhydrazine. Photoelectrochemical and photoluminescence confirm that 3 wt% Bi 2 Sn 2 O 7 /Bi 5 O 7 I composites exhibit the highest separation rate of photogenerated carriers. Finally, based on the results of experimental studies and theoretical calculations, the S-scheme charge transfer path on Bi 2 Sn 2 O 7 /Bi 5 O 7 I composite is determined. This work provides a new perspective on how to design high-performance S-scheme bismuth oxyhalide-based heterojunction photocatalysts for solar energy conversion.
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POLYMER
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2024
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IF 4.1
Chunlei Xu,Hang Guo,Changzhu Lv,Wei Chen,Liangbin Li,Kunpeng Cui
Understanding on the structure and dynamics of poly(vinyl acetal)s is insufficient due to the complicated chemical structure and amorphous nature of this type of polymers. In this work, we investigate the effect of side group length on structure and dynamics heterogeneity at different length scales spanning from side group, segment, and polymer network by combing dynamic mechanical analysis (DMA), dielectric relaxation spectroscopy (DRS), solid-state NMR, and differential scanning calorimetry analysis (DSC). By increasing the length of acetal side group, its intrinsic dynamics slows down. Taking into account the scale of segment and networks, with the increase of acetal group length, the formation of cross-linking sites formed by the hydroxyl-rich domain is suppressed, the relaxation distribution of the segment widens, and the volume fraction of rigid component decreases. The effect of side group length on the structure and dynamics heterogeneity of poly(vinyl acetal)s at different scales results in significant changes in material properties such as the non-monotonic change in loss factor value (tan δ ) and a monotonous reduction in glass transition temperature ( T g ).
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Cell Reports
·
2024
·
IF 7.5
Mingzhi Wu,Xiaojun Zhou,Xinyi Zhou,Genxin Wang,Yiqun Zeng,Jun Li,Edward V. Prochownik,Fubing Wang,Youjun Li
Cholesterol metabolism reprogramming plays essential roles in hepatocellular carcinoma (HCC). However, precisely how cholesterol metabolism is dysregulated is not clear. Here, we show that the palmitoyltransferase ZDHHC3 and depalmitoylase ABHD17A regulate HCC cell cholesterol biosynthesis by dynamically S-acylating SREBP cleavage-activating protein (SCAP). SCAP S-acylation by ZDHHC3 at C264 antagonizes HACE1-mediated SCAP ubiquitination. Intriguingly, SREBP2 transcriptionally upregulates ZDHHC3 to form a positive feedback loop, which explains why negative feedback regulation of SCAP/SREBP2 signaling fails in HCC. Increased cholesterol in the tumor microenvironment (TME) restrains CD4 + T cell cytotoxicity. Hence, the cholesterol metabolism reprogramming and cholesterol level alternation in the TME cooperate to promote HCC development. We identified a small-molecule inhibitor of ZDHHC3 that, combined with anti-PD-1 immunotherapy, inhibited diethyl nitrosamine (DEN)/CCl 4 -induced HCC growth in mice. ZDHHC3-mediated SCAP S-acylation reprograms cholesterol metabolism and promotes HCC immune escape. ZDHHC3 is thus identified as a rational chemotherapy target for HCC.
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2024
·Vol. 26
·期 29
·19658-19672
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IF 2.9
Yaqi Liu,Guicheng Luo,Yichen Liu,Zuozheng Xu,Hengxin Shen,Yuxiang Sheng,Yuan Zhu,Shuyi Wu,Lizhe Liu,Yun Shan
Photocatalytic degradation of organic pollutants in water is of great significance to the sustainable development of the environment, but encounters limited efficiency when a single compound is used. Thus, there have been enormous efforts to find novel photocatalytic heterostructured composites with high performance. In this work, a novel S-scheme heterostructure is constructed with BiOBr and Zn2+ doped C4N3 (Zn–C4N3) by a solvothermal method for efficient photodegradation of tetracycline (TC), a residual antibiotic difficult to be removed from the aquatic environment. Thanks to Zn2+-doping induced improvement in chemical affinity between Zn–C4N3 and BiOBr, well-formed Zn–C4N3/BiOBr heterostructured hollow spheres are formed. This structure can efficiently suppress fast recombination of photogenerated electron–hole pairs to enhance the photocatalytic activity of BiOBr dramatically. At a room temperature of 25 °C and neutral pH 7, the catalyst can degrade a significant portion of TC pollutants within 30 min under visible light. Also, the Zn–C4N3/BiOBr heterostructure displays good stability after recycling experiments. Free radical capture experiments and ESR tests show that ˙O2− is the main active substance for photocatalytic degradation of TC. This study provides new insights for constructing heterostructures with an intimate interface between the two phases for photocatalytic applications.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Hongwu Liao,Chong Wang,Jiaxian Zheng,Zhuo Chen,Yulin Zhou,Chengning Ye,Xiangfeng Lin,Meng An,Yusuke Yamauchi,Yusuke Asakura,Zhanhui Yuan
Photocatalytic depolymerization of lignin offers a sustainable approach to producing high-value-added aromatic compounds. Recently, carbon nitride has demonstrated notable selectivity for the C C bonds in lignin model compounds. However, limitations of pure carbon nitride include the low mobility of photogenerated electrons and the difficulty in precisely controlling the cleavage pathways and products of C C bonds. In this study, we constructed an S-Scheme heterojunction by in situ loading of Ce ions onto C 3 N 4 to form a CeO 2 /C 3 N 4 composite. This heterojunction achieves efficient lignin depolymerization under blue LED irradiation in an oxygen-rich environment. Comparative analysis indicated that the yield of primary products, benzaldehyde and phenyl formate, increased by 7.8-fold and 7.75-fold, respectively, compared with pure CeO 2 , and by 1.4 and 1.8 times relative to unmodified C 3 N 4 . After optimizing the reaction conditions, dealkalized lignin is applied to the system and successfully depolymerized. Comprehensive characterization and theoretical simulations verify the heterojunction's ability to enhance carrier separation and redox activity, with CeO 2 serving as an active dehydrogenation site that significantly boosts the depolymerization efficiency of lignin model compounds. This photocatalytic strategy presents a valuable step forward in lignin valorization and supports the sustainable utilization of biomass resources.
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Small
·
2024
·
IF 13
Shikai Wang,Dong Zhang,Xipeng Pu,Lizhi Zhang,Dafeng Zhang,Jizhou Jiang
Herein, guided by the results of density functional theory prediction, the study rationally designs a hollow core–shell FeNi 2 S 4 @ZnIn 2 S 4 (FNS@ZIS) Step-scheme (S-scheme) heterojunction for photocatalytic H 2 evolution with photothermal-assisted. The hollow FNS spheres offered substrate for coating the ZIS nanosheets, which can inhibit ZIS nanosheets from agglomerating into pellet, enrich the active site, increase specific surfaces, and raise the light absorption. Notably, due to its excellent photothermal properties, FNS core generated heat unceasingly inside under visible-light irradiation and effectively prevent the heat loss of the reaction system, which increased the local temperature of photocatalysts and thus accelerated the charge migration. In addition, the S-scheme heterojunction construction via in situ growth has a tight interface, which can facilitate the separation and transfer of carriers and achieve high redox potential. Owning to the distinctive construction, the hollow core–shell FNS@ZIS S-scheme heterojunction show extraordinary stability and photocatalytic H 2 evolution rate with 7.7 mmol h −1 g −1 , which is ≈15.2-fold than pristine ZIS. Based on the double evidence of theoretical predictions and experimental confirmations, the photothermal effect and electron transfer mechanism of this innovative material are investigated in depth by the following infrared thermography technology and deep DFT calculations.
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MOLECULES
·
2024
·Vol. 29
·期 9
·1931
·
IF 4.2
Yuhong Lin,Zhuoyuan Chen,Chang Feng,Li Ma,Jiangping Jing,Jian Hou,Likun Xu,Mingxian Sun,Dongchu Chen
In this study, S-doped graphitic carbon nitride (S-C3N4) was prepared using the high-temperature polymerization method, and then S-C3N4/AgCdS heterojunction photocatalyst was obtained using the chemical deposition method through loading Ag-doped CdS nanoparticles (AgCdS NPs) on the surface of S-C3N4. Experimental results show that the AgCdS NPs were evenly dispersed on the surface of S-C3N4, indicating that a good heterojunction structure was formed. Compared to S-C3N4, CdS, AgCdS and S-C3N4/CdS, the photocatalytic performance of S-C3N4/AgCdS has been significantly improved, and exhibits excellent photocatalytic degradation performance of Rhodamine B and methyl orange. The doping of Ag in collaboration with the construction of a Z-scheme heterojunction system promoted the effective separation and transport of the photogenerated carriers in S-C3N4/AgCdS, significantly accelerated its photocatalytic reaction process, and thus improved its photocatalytic performance.
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Advanced Energy Materials
·
2020
·Vol. 10
·期 25
·1904026
·
IF 25.245
Wenqiang Wang,Dongya Wang,Guiyou Wang,Mengyao Zheng,Gengchao Wang
The shuttle of polysulfide and severe volume change of sulfur cathodes, are the bottlenecks in the practical application of lithium–sulfur batteries, and need to be solved through further exploration of simple and scalable strategies. Herein, an elastic and conductive coating layer is designed and synthesized, by combining water soluble conducting polymer modified carbon nanotubes (PASANTs) with crosslinked waterborne polyurethane ( c WPU). It shows high electronic conductivity and excellent resilience. As a result, a lithium–sulfur battery with c WPU/PASANTs coated cathode is able to achieve an outstanding cycle stability with a capacity of 70.8% after 500 cycles at 0.5C and an excellent rate performance (specific capacity of 1130 mAh g −1 at 0.1C and maintain 68.2% at 2C). This work embodies a systematic design concept, which shows the application prospects of large-scale production, and is expected to be further applied to other easily pulverized high-specific-capacity materials such as silicon and tin.
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