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APPLIED CATALYSIS B-ENVIRONMENTAL · 2024 · IF 20.2

Positive feedback of intermediates promotes efficient electrocatalytic C-N coupling at AuPd/SnOx interfaces

Hua Wang,Yunchuan Tu,Sijun Li,Yimin Jiang,Niandan Zhao,Wenbin Wang,Wei Shen,Ming Li,Rongxing He

Efficient electrocatalytic co-reduction of CO 2 and NO 3 − to urea involves simultaneous generation and stabilization of C- and N-coupling intermediates. Herein, we report positive feedback at the interfaces of an AuPd/SnO x catalyst that enables generation and stable co-adsorption of *CO and *NH 2 OH at low-potential, fostering efficient C-N coupling for urea formation. A combination of in-situ spectroscopic analyses and theoretical calculations show that *CO 2 captures electrons by bonding to the AuPd/SnO x interface, leading to positively charged Pd sites, which promote the NO 3 RR to give the key N-intermediate *NH 2 OH. The adsorbed *NH 2 OH provides electron feedback to the catalyst surface , which not only enhances the adsorption of CO 2 and promotes the conversion of *CO 2 to *CO to accelerate the CO 2 RR, but also enhances the adsorption strength of the catalyst for *CO. Owing to this positive feedback, the Faraday efficiency and yield of urea reached 21.3 % and 1280.5 μg∙h −1 ∙mg −1 at −0.2 V (versus the relative hydrogen electrode), surpassing the performance of most previously reported catalysts. This finding provides new insights into catalyst design for advancing C-N coupling systems.

研究领域: 化学 · 材料科学 · 催化反应
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MOLECULAR PHARMACEUTICS · 2019 · IF 4.396

Reduced Toxicity of Liposomal Nitrogen Mustard Prodrug Formulation Activated by an Intracellular ROS Feedback Mechanism in Hematological Neoplasm Models

Mengting Lin,Wangwei Guo,Zhentao Zhang,Yi Zhou,Jiejian Chen,Tiantian Wang,Xincheng Zhong,Yiying Lu,Qiyao Yang,Qichun Wei,Min Han,Donghang Xu,Jianqing Gao

Nitrogen mustard (NM) is among the earliest drugs used to treat malignant tumors and it kills tumor cells by cross-linking DNA. Unfortunately, because of the short half-life and unfavorable selectivity, NM causes significant damage to normal tissues. As NM can increase the levels of reactive oxygen species (ROS) in tumor cells, a ROS-activated nitrogen mustard prodrug (NM-Pro) was synthesized and mixed with NM at a specific ratio to obtain an “NM-ROS-NM-Pro-NM” positive feedback system, which ultimately achieves a specific lethal effect on hematological neoplasms. The further encapsulation of NM/NM-Pro in liposomes allows the sustained release of the drug and prolongs the residence time in vivo. Here, we prepared stable liposomes with a uniform particle size of 170.6 ± 2.2 nm. The optimal ratio of NM to NM-Pro in this study was 2:1. The active drug NM in the NM/NM-Pro system continuously stimulated ROS production by the cells, which in turn further activated the NM-Pro to continuously generate NM. The positive feedback pathway between the NM and NM-Pro resulted in the specific death of tumor cells. Furthermore, the K562 hematological neoplasm model was utilized to evaluate the therapeutic effect of NM/NM-Pro liposomes in vivo. After encapsulation in liposomes, the targeting of tumor cells was increased approximately two times compared with that of normal cells, and NM/NM-Pro liposomes exhibited reduced toxicity, without an increase in drug activity compared to the NM/NM-Pro combination. The NM/NM-Pro delivery system exerts a positive feedback effect on ROS production in tumor cells and displays good potential for the specific killing of hematoma cells.

CAS / MDL: 1000342-11-9
研究领域: 肿瘤学 · 药理学 · 分子生物学
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ATMOSPHERIC ENVIRONMENT · 2024 · IF 4.2

A light - Driven acidic positive feedback mechanism of sulfate formation

Chunyan Zhang,Qingxin Ma,Peng Zhang,Tianzeng Chen,Yonghong Wang,Biwu Chu,Hao Li,Jikun Li,Chuncheng Chen,Jincai Zhao,Hong He

As the main source of atmospheric sulfate aerosol , the aqueous-phase oxidation of SO 2 has been of great concern. Traditionally, the aqueous-phase oxidation of SO 2 is considered a consumption process of atmospheric oxidation capacity; however, we report here that •OH radicals and other reactive oxygen species (ROS) can be generated in the photochemical reactions of bulk HSO 3 − solution. This •OH production pathway results in the fast sulfate formation in the photooxidation of dissolved SO 2 . The photochemical process is determined to be pH-dependent in which sulfate formation is promoted by decreasing pH. Hence, a light - driven acidic positive feedback mechanism is proposed that the oxidation of dissolved SO 2 and the formation of •OH radicals have a synergistic promoting effect. These results indicate that the photochemistry of dissolved SO 2 could be a missing source of aqueous •OH radicals as well as sulfate at regional to global scales.

研究领域: 大气科学 · 环境化学
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ADVANCED FUNCTIONAL MATERIALS · 2025 · IF 19

Closed-Loop Responsive Smart Bandages for Dynamic Monitoring and Self-Regulated Antibacterial Therapy in Wound Healing

Zhaochuan Yu,Chao Deng,Liucheng Meng,YiJin Wang,Chengcheng Li,Chao Liu,Yuqian Liu,Farzad Seidi,Xing Zhang,Qiang Yong,Hao Wu,Huining Xiao

Currently, smart wound management systems have garnered increasing attention. However, most existing strategies still rely on predefined stimuli or threshold-based mechanisms to trigger drug release, which are insufficient to feedback to the dynamic changes in infection status, and their independently designed sensing and therapeutic modules further limit functional integration and coordinated intervention. To address these challenges, this study presents a smart bandage system that integrates a closed-loop mechanism encompassing sensing, therapy intervention, and feedback. The system is built by embedding carbon dots (CDs) into metal–organic frameworks (MOFs) formed via Fe 3+ -carbenicillin (CARB) coordination, then immobilized on a cellulose nonwoven (CNW) to create a composite smart bandage. In the infection-induced acidic microenvironment, the bandage enables concurrent fluorescence recovery and CARB release, enabling real-time infection monitoring and potent antibacterial activity (>99.99%). As infection resolves, diminished bacterial activity raises local pH, thereby reducing CARB release through pH-responsive negative feedback. Mechanistic studies indicate that Fe 3+ competitively coordinates between bacterial ligands and CDs, enabling coupled sensing and therapy. In a murine wound model, the bandage significantly accelerated wound healing, suppressed bacterial growth, and allowed visual tracking of infection severity. This work provides a novel strategy for an intelligent wound bandage with autonomous sensing and therapeutic functions.

CAS / MDL: 9002-89-5
研究领域: 生物医学工程 · 智能材料 · 伤口护理 · 纳米医学 · 抗菌治疗
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ACS Applied Materials & Interfaces · 2020 · IF 8.758

Biodegradable Multifunctional Nanotheranostic Based on Ag2S-Doped Hollow BSA-SiO2 for Enhancing ROS-Feedback Synergistic Antitumor Therapy

Ziliang Zheng,Rong Dai,Zhuo Jia,Xiaorong Yang,Yufei Qin,Shuo Rong,Xiaoyang Peng,Xianmei Xie,Yanyan Wang,Ruiping Zhang

Stimuli-responsive silica nanoparticles are an attractive therapeutic agent for effective tumor ablation, but the responsiveness of silica nanoagents is limited by intrastimulation level and silica framework structure. Herein, a biodegradable hollow SiO2-based nanosystem (Ag2S-GOx@BHS NYs) is developed by a novel one-step dual-template (bovine serum albumin (BSA) and cetyltrimethylammonium bromide (CTAB)) synthetic strategy for image-guided therapy. The Ag2S-GOx@BHS NYs can be specifically activated in the tumor microenvironment via a self-feedback mechanism to achieve reactive oxygen species (ROS)-induced multistep therapy. In response to the inherent acidity and H2O2 at the tumor sites, Ag2S-GOx@BHS would accelerate the structural degradation while releasing glucose oxidase (GOx), which could efficiently deplete intratumoral glucose to copious amounts of gluconic acid and H2O2. More importantly, the sufficient H2O2 not only acts as a reactant to generate Ag+ from Ag2S for metal-ion therapy and improves the oxidative stress but also combines with gluconic acid results in the self-accelerating degradation process. Moreover, the released Ag2S nanoparticles can help the Ag2S-GOx@BHS NYs realize the second near-infrared window fluorescence (NIR-II FL) and photoacoustic (PA) imaging-guided precise photothermal therapy (PTT). Taken together, the development of a self-feedback nanosystem may open up a new dimension for a highly effective multistep tumor therapy.

研究领域: 纳米技术 · 癌症治疗 · 材料科学 · 生物医学工程 · 诊疗学
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