ENERGY & FUELS
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2025
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IF 5.3
Yanmei Zhao,Yafang Zhao,Jun Zheng,Yueying Lin,Chuanfang Liu,Jiafan Zheng,Chengyu Zhang,Kai Zhang,Zhongrong Shen
Hydrothermal carbonization of sucrose is a conventional method for preparing hard carbon (HC) microsphere precursors; the construction of closed pores plays a crucial role in enhancing the platform capacity of sugar-based HC materials. This work proposes a strategy of a cohydrothermal method with sucrose and organic amine molecules to regulate the content of closed pores. Amine molecules undergo an amine-aldehyde condensation reaction with furfural intermediates during the hydrothermal process of sucrose, participating in the formation of carbon precursors. During the carbonization process, the presence of amine molecules accelerates the pyrolysis of the precursor and alters the microstructure of the HC microsphere precursor. This ultimately leads to the construction of closed pore structures during subsequent carbonization, thereby significantly enhancing the platform capacity. Research finds that different amine molecules affect the sodium ion storage behavior of the HC anode materials. Specifically, aniline-involved sucrose-derived HC (HCBS) and benzylamine-involved sucrose-derived HC (HCBIS) deliver large closed-pore volume of 0.072 m3 g–1 and 0.095 m3 g–1, respectively, much higher than sucrose-derived HC (HCS) of 0.024 m3 g–1. HCBS exhibits a remarkable reversible capacity of 382 mA h g–1 at a current density of 0.020 A g–1. Ex situ Raman tests demonstrate that the plateau capacity of HCBS (277 mA h g–1) results from both sodium ion intercalation and closed pore filling; conversely, the plateau capacity of HCBIS is primarily attributed to closed-pore filling. This work proposes a novel design concept to create abundant closed pores HC from sucrose, contributing to the rational design of the pore structure of sugar-based HC.
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ACTA PHYSICO-CHIMICA SINICA
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2025
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IF 13.5
Yi Yang,Xin Zhou,Miaoli Gu,Bei Cheng,Zhen Wu,Jianjun Zhang
Photocatalytic hydrogen peroxide (H 2 O 2 ) production is a crucial process for clean energy conversion, involving the reduction of O 2 through two electrons. However, this process is often hampered by the sluggish water oxidation involving the photogenerated holes. To address this challenge, we have constructed a dual-functional S-scheme ZnO/CdIn 2 S 4 heterojunction systerm coupling the H 2 O 2 generation with a value-added benzylamine (BA) oxidation reaction. In this dual-functional photocatalytic system, photogenerated electrons in CdIn 2 S 4 efficiently reduce O 2 to produce H 2 O 2 , while photogenerated holes in ZnO selectively oxidize BA to N-benzylidenebenzylamine. Leveraging the advantages of the S-scheme heterojunction, the optimized ZnO/CdIn 2 S 4 photocatalyst displays an enhanced H 2 O 2 production rate (386 μmol·L −1 ·h −1 ) and BA oxidation fraction (81%) than pure ZnO or CdIn 2 S 4 . Femtosecond transient absorption (fs-TA) spectroscopy confirm the ultrafast S-scheme electron transfer from the ZnO conduction band (CB) to the CdIn 2 S 4 valence band (VB) upon photoexcitation of the ZnO/CdIn 2 S 4 composite. Besides, timely depletion of VB holes in ZnO and CB electrons in CdIn 2 S 4 can accelerate the interfacial electron transfer in the ZnO/CdIn 2 S 4 S-scheme heterojunction. The innovative design of the ZnO/CdIn 2 S 4 S-scheme photocatalyst provides new insights for developing efficient dual-functional heterojunction photocatalytic systems and introduces a novel method for studying S-scheme heterojunctions using fs-TA spectroscopy.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Liyi Tang,Yangsen Xu,Shuang Tang,Yu-Xiang Yu,Aiyun Meng,Xinzhong Wang,Wei-De Zhang
Photocatalytic hydrogen production utilizing solar energy provides a pivotal strategy for realizing a carbon–neutral society. Cocatalyst-modified semiconductor materials have emerged as promising candidates for photocatalytic applications due to their ability to facilitate the spatial separation and directional migration of photogenerated electron-hole pairs. Nevertheless, those systems often face challenges such as intricate preparation procedures and issues with non-compact recombination. Herein, we report a one-pot thermal treatment approach for synthesizing a composite of Mn 3 O 4 nanoparticles and sodium poly(heptazine imides) (Na-PHI). Mn 3 O 4 nanoparticles were in situ generated and embedded within the Na-PHI matrix during the sintering process. The resulted photocatalyst demonstrated significantly enhanced photoinduced charge separation efficiency, exhibiting approximately 6-fold and 3-fold improvements compared to pristine Mn 3 O 4 and Na-PHI, respectively. The photocatalytic hydrogen evolution rate reached 14 μmol h −1 , nearly 14 times that of Na-PHI (1.2 μmol h −1 ) in the aqueous solution of benzylamine (BA) under visible light illumination (780 nm ≥ λ ≥ 420 nm). Furthermore, the optimized Mn 3 O 4 -Na-PHI sample (Mn-Na-PHI) displayed a remarkably high photocatalytic hydrogen generation rate alongside the synchronous photo-oxidative coupling of aliphatic and aromatic amine under visible light. This work underscores the potential for rational design and synthesis of novel Na-PHI-based functional composites for sustainable energy applications.
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NANO LETTERS
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2025
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IF 9.1
Aumber Abbas,Qian Zhang,Jamal Kazmi,Ying Li,Wenbo Li,Waqas Ahmad,Chao Zou,Qijie Liang
Chiral discrimination is crucial in chiral synthesis, pharmaceuticals, and biology. Although surface-enhanced Raman scattering (SERS) provides highly sensitive molecule-specific vibrational data, existing approaches depend on indirect detection involving supplementary selectors, impeding clear and versatile chiral discrimination. Here, we report the direct label-free SERS sensing of different biologically prominent enantiomers with a two-dimensional transition metal dichalcogenide, such as TaS2, based chiral superlattice to produce enantiospecific molecular fingerprints. The clear enantiodiscrimination between a model chiral pair of l- and d-glucose is achieved with a detection limit of 8 × 10–10 M. In addition, noninvasive identification of l- and d-glucose in actual saliva samples and multiplex quantification of enantiomeric ratios with superior predictive accuracy are accomplished.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-10
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IF 15.7
Fan Yun,Yan Yunhui,An Qizheng,Xia Zhongcheng,Pan Yuping,Lu Yuxuan,Zhu Zhonghuan,Wang Ruiqi,Liu Qinghua,Zou Yuqin,Li Yongjun,Wang Shuangyin
The use of renewable electricity to drive the electrocatalytic coupling of CO with nitrogen-containing organics offers a promising strategy for producing high-value chemicals. In this work, we conduct a systematic investigation of the coordination effect between iodide and copper oxide to generate Cu δ+ active sites. These Cu δ+ sites enable the electrosynthesis of dimethylacetamide from CO and dimethylamine. Through precise regulation of the electrode surface microenvironment, a dimethylacetamide Faradaic efficiency of 45.6% is achieved at a partial current density of 182.4 mA·cm -2 , with a production rate of 435.9 mmol·g cat. −1 ·h -1 and selectivity approaching 70%. Mechanistic studies reveal that specific adsorption of I - forms an iodide-enriched Cu 0 /Cu + interface that synergistically promotes dimethylacetamide formation by enhancing adsorption of ketene intermediates (*CCO) and facilitating C–N bonds formation. This anion-coordination interfacial engineering strategy demonstrates broad applicability for synthesizing various acetamide derivatives from CO 2 /CO and amine, providing a foundational framework for electrocatalytic C-N coupling in acetamide synthesis.
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JOURNAL OF PHOTOPOLYMER SCIENCE AND TECHNOLOGY
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2025
·Vol. 38
·期 1
·11-19
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IF 0.7
Mengting Zhao,Mengyun Wang,Li Jin,Boyang Cheng,Tianjiao Hou,Xuan Shen
The development of high-performance UV-LED excited photoinitiators (PIs) is one of the current research hot spots in the field of photopolymerization. Thioxanthone (TX) derivatives have good UV-visible absorption ability under UV excitation. In this article, four novel thioxanthone derivatives were designed and synthesized as one-component polymerizable photoinitiators, and their structures were confirmed by FT-IR and 1H NMR. Their photophysical/photochemical, kinetic and migration stability were investigated experimentally by UV-vis spectrophotometer and Fourier transform infrared spectrometer. The photolysis and photoinitiation mechanisms of four initiators were elucidated. Comparison of the results for the TX system showed that these TX derivatives are highly efficient one-component polymerizable PIs with high migration stability, which has the potential to be used in UV curing systems, especially for food packaging and biomedical applications.
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Journal of Materials Chemistry A
·
2025
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IF 9.5
Lele Wang,Weiran Wu,Wenpeng Zhang,Xinlei Ren,Xuan Liu,Wing-Kei Ho,Jie Hu,Min Zhou
Photocatalytic hydrogen peroxide (H2O2) production using resorcinol-formaldehyde (RF) resin offers a sustainable strategy, but its efficiency is limited by high exciton binding energy, suppressing free charge carriers generation. Herein, an S-scheme heterojunction composed of RF and MgIn2S4 (RF/MIS) was constructed to minimize exciton binding energy by modulating charge transfer pathways. The well-designed S-scheme charge transfer mechanism facilitates photoexcited carrier separation, strengthening redox capability driven by the interfacial electric field. In situ irradiation X-ray photoelectron spectroscopy, temperature-dependent photoluminescence, and photoelectrochemical measurements reveal that the reduced exciton binding energy leads to enhanced oxygen reduction efficiency. The optimized RF/MIS achieves significant H2O2 production rates of 892.6 μmol·L-1·h-1 under full-spectrum (320-780 nm), specifically producing 18.2 μmol·L-1·h-1 of H2O2 under 730 nm irradiation, along with superior stability in consecutive recycling tests. The two-electron reduction mechanism is evidenced by electron paramagnetic resonance spectroscopy and rotating ring-disk electrode analysis. These findings establish fundamental connections between heterointerface-trapped exciton dynamics and photocatalytic efficiency, providing new directions for designing high-performance organic semiconductors.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
·
IF 9.7
Tao Guo,Danjun Mao,Xiufeng Lu,Wenhao Ma,Heyun Fu,Huan He,Cheng Sun,Shourong Zheng,Zhifeng Jiang,Xiaolei Qu
Inadequate contact interface, lack of direct electron-transfer paths and low substrate affinity are considered as the main obstacle inhibiting the heterostructure activity for the sustainable photosynthesis of value-added fine chemicals. Herein, a novel 0D/2D Step-scheme (S-scheme) α-Fe 2 O 3 /PbBiO 2 I (FO/PBOI) composite with abundant interface Fe O bonds were initially synthesized via an in-situ growth approach. The created built-in field as a powerful driving force, efficiently steering the migration of photogenerated electrons. The interfacial Fe O bonds act as atomic-level transfer highway, lowering charge transfer energy barrier between the interfaces and further accelerating the S-scheme spatial charge separation. Moreover, the Fe O bonds bridged FO/PBOI can effectively enhance the activation of O 2 and benzylamine, significantly reducing the dehydrogenation barrier for the rate-limiting C 6 H 5 CH 2 NH* intermediate. The optimized FO/PBOI exhibits remarkably improved catalytic activity and general applicability for the dehydrocoupling of primary amines to imines. This work offers an atomic-scale perspective on precise charge flow steering based on interface bond for advanced organic transformations.
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Journal of Materials Chemistry A
·
2025
·
IF 9.5
Jiani Yang,Chao Xiong,Mi Zhou,Xianglin Luo,Xikui Liu,Chong Cheng,Chao He,Xiaohui Xu
Considering the intrinsic limitations of natural enzymes, the development of efficient, cost-effective artificial enzyme alternatives has become imperative. Covalent metal-organic frameworks (CMOFs), as a new type of open framework materials with precise crystalline structures, clear metal catalytic sites, ordered pores and strong designability, can be considered as an ideal platform to develop efficient artificial enzyme materials. Here, we report two distinct enzyme-mimetic CMOFs, Tbpa-Ag3 and Tbpa-Cu3, which featured cyclic trinuclear metal clusters (Ag3/Cu3) as functional nodes respectively. Among the two CMOFs, Tbpa-Ag3 achieved precise spatial integration of photoactive Tbpa ligands with catalytic Ag3 clusters, establishing a more efficient electron transfer pathway that delivered superior oxidase-like activity under visible-light irradiation. Based on Tbpa-Ag3, we engineered a biomarker detection platform for physiological antioxidants (L-Cysteine and GSH) and a sustainable photocatalytic system for benzylamine oxidative coupling (yield > 99%, 4 h), validating Tbpa-Ag3’s dual functionality in analytical chemistry and green catalysis.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Xiaolu Zhou,Honggang Zhang,Jiari He,Difei Xiao,Zeyan Wang,Peng Wang,Zhaoke Zheng,Hefeng Cheng,Ying Dai,Baibiao Huang,Yuanyuan Liu
While various strategies, such as introducing n-π* transitions and expanding π-conjugated systems, have been proven to effectively enhance light harvesting for metal-organic frameworks (MOFs), their practical application is often hampered by ligand structure dependency—specifically, the requirement for complex ligand synthesis. To address this limitation, this work reports an in-situ ligand hydroxylation strategy during the synthesis of Bi-based MOFs. This approach not only broadens the light absorption range of the MOFs but also circumvents environmentally unfriendly synthetic conditions (e.g., high temperature or strong oxidants). This phenomenon is first observed in BDC-(OH) 2 containing two hydroxyl groups, which is transformed to BDC-(OH) 4 with four hydroxyl groups in the final MOF, denoted as Bi-BDC-(OH) 4 , as directly seen in the single crystal structure. Furthermore, the in-situ hydroxylation process is successfully extended to other ligands, including gallic acid (GA) and quercetin (QC), demonstrating its universality. Importantly, the hydroxylation also increases the charge separation efficiency of Bi-BDC-(OH) 4 . This work provides a novel and practical strategy to enhance light utilization and improve the photocatalytic efficiency of Bi-based MOFs.
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