摘要：
Achieving fast transmembrane transmission of molecules in organisms is a challenging problem. Inspired by the transport of Dopmine (DA) in organisms, the DA transporter (DAT) binds to DA in a way that has a ring recognition (the recognition group is the tryptophan group). Herein, D-Tryptophan-pillar[5]arene (D-Trp-P5) functionalized conical nanochannel is constructed to achieve fast transmission of DA. The D-Trp-P5 functionalized nanochannel enables specific wettability recognition of DA molecules and has great cycle stability. With the controlling of voltage to wettability, the transport flux of DA is up to 499.73 nmol cm(-2) h(-1) at -6 V, 16.88 times higher than that under positive voltages. In response to these results, a high-throughput DA transport device based on controlled electricity-wettability is provided.
通讯机构：
[Zhang, AD ] C;Cent China Normal Univ, Minist Educ, Coll Chem, Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.
摘要：
We report herein a dynamic facet-selective capping (dFSC) strategy for α-calcium sulfate hemihydrate crystal growth from dihydrate gypsum in the presence of a catechol-derived PEI capping agent (DPA-PEI) with inspiration by the biomineralization process of mussel. The crystal shape is controllable and varies from long and pyramid-tipped prisms to thin hexagonal plate. The highly uniform truncated crystals have extremely high compression and bending strengths after hydration molding.
摘要：
Semiconductor-based photoelectrochemical (PEC) biosensors have garnered significant attention in the field of disease diagnosis and treatment. However, the recognition units of these biosensors are mainly limited to bioactive macromolecules, which hinder the photoelectric response due to their insulating characteristics. In this study, we develop an in situ-sensitized strategy that utilizes a small-molecule probe at the interface of the photoelectrode to accurately detect α-glucosidase (α-Glu) activity. Silane, a prototype small-molecule probe, was surface-modified on graphitic carbon nitride to generate Si nanoparticles upon reacting with hydroquinone, the enzymatic product of α-Glu. The in situ formed heterojunction enhances the light-harvesting property and photoexcited carrier separation efficiency. As a result, the in situ-sensitized PEC biosensor demonstrates excellent accuracy, a low detection limit, and outstanding anti-interference ability, showing good applicability in evaluating α-Glu activity and its inhibitors in human serum samples. This novel in situ sensitization approach using small-molecule probes opens up new avenues for developing simple and efficient PEC biosensing platforms by replacing conventional biorecognition elements.
摘要：
Tudor domain-containing protein 3 (TDRD3) is involved in regulating transcription and translation, promoting breast cancer progression, and modulating neurodevelopment and mental health, making it a promising therapeutic target for associated diseases. The Tudor domain of TDRD3 is essential for its biological functions, and targeting this domain with potent and selective chemical probes may modulate its engagement with chromatin and related functions. Here we reported a study of TDRD3 antagonist following on our earlier work on the development of the SMN antagonist, Compound 1, and demonstrated that TDRD3 can bind effectively to Compound 2, a triple-ring analog of Compound 1. Our structural analysis suggested that the triple-ring compound bound better to TDRD3 due to its smaller side chain at Y566 compared to W102 in SMN. We also revealed that adding a small hydrophobic group to the N-methyl site of Compound 1 can improve binding. These findings provide a path for identifying antagonists for single canonical Tudor domain-containing proteins such as TDRD3 and SMN.
摘要：
Inspired by ion pair cotransport channels in biological systems, a bionic nanochannel modified with lithium ion pair receptors is constructed for selective transport and enrichment of lithium ions (Li(+)). NH(2)-pillar[5]arene (NP5) is chosen as ion pair receptors, and the theoretical simulation and NMR titration experiments illustrate that NP5 has good affinity for the ion pair of LiCl through a strong host-guest interaction at the molecular level. Due to the confinement effect and ion pair cooperation recognition, an NP5-based receptor was introduced into an artificial PET nanochannel. An I-V test indicated that the NP5 channel realized the highly selective recognition for Li(+). Meanwhile, transmembrane transport and COMSOL simulation experiments proved that the NP5 channel achieved the transport and enrichment of Li(+) through the cooperative interaction between NP5 and LiCl. Moreover, the receptor solution of transmembrane transport LiCl in the NP5 channel was used to cultivate wheat seedlings, which obviously promoted their growth. This nanochannel based on the ion pair recognition will be much useful for practical applications like metal ion extraction, enrichment, and recycle.
作者机构：
[Xu, Guang; Chen, Jian; Yu, Hong; Liu, Jinpeng; Yin, Tingrui; Meng, Sixuan; Zhang, Ying; Yu, Guang-Ao] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensor Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.;[Lin, Xiuhua; Dang, Li; Dang, L] Shantou Univ, Dept Chem, Shantou 515063, Guangdong, Peoples R China.;[Lin, Xiuhua; Dang, Li; Dang, L] Shantou Univ, Key Lab Preparat & Applicat Ordered Struct Mat Gua, Shantou 515063, Guangdong, Peoples R China.;[Lin, Xiuhua; Dang, Li; Dang, L] Chem & Chem Engn Guangdong Lab, Shantou 515063, Guangdong, Peoples R China.;[Yuan, Jia; Yuan, J] Wuhan Text Univ, State Key Lab New Text Mat & Adv Proc Technol, Wuhan 430200, Peoples R China.
通讯机构：
[Yuan, J ] W;[Yu, GA ] C;[Dang, L ] S;Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensor Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.;Shantou Univ, Dept Chem, Shantou 515063, Guangdong, Peoples R China.
摘要：
We developed the remote selective C-H bromination for the synthesis of C4 & PRIME;-brominated biarylphosphine oxides using FeBr3 as a brominating reagent. C3 & PRIME;-Brominated products were obtained in reactions with substrates bearing a 2,4,6-triisopropyl substituent on the bottom ring. Moreover, direct access to C5-chlorinated peri-substituted(1-naphthalenyl)phosphines is developed using FeCl3 as a chlorinating reagent. These halogenated compounds can be utilized for cross-coupling reactions to construct functionalized phosphine oxides.
作者机构：
[Canete, Pablo F.; Wang, Runli; Yao, Yin; Yunis, Joseph; Chen, Zhian; Wang, Naiqi; Davis, David Simon; Yu, Di; Yu, Zhijia; Wang, Hao] Univ Queensland, Frazer Inst, Fac Med, Brisbane, Qld, Australia.;[Wang, Runli; Yao, Yin; Yunis, Joseph; Roco, Jonathan A.; Gao, Xin; Chen, Zhian; Davis, David Simon; Yu, Di; Parish, Christopher; Yu, Zhijia; Wang, Hao] Australian Natl Univ, John Curtin Sch Med Res, Canberra, ACT, Australia.;[Cui, Yanfang] Cent China Normal Univ, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan, Peoples R China.;[Yao, Yin; Liu, Zheng] Huazhong Univ Sci & Technol, Tongji Hosp, Tongji Med Coll, Dept Otolaryngol Head & Neck Surg, Wuhan, Peoples R China.;[Qi, Hai; Liu, Bo] Tsinghua Univ, Tsinghua Peking Ctr Life Sci, Sch Med cine, Lab Dynam Immunobiol, Beijing, Peoples R China.
摘要：
In antibody responses, mutated germinal center B (BGc) cells are positively selected for reentry or differentiation. As the products from GCs, memory B cells and antibody-secreting cells (ASCs) support high-affinity and long-lasting immunity. Positive selection of BGc cells is controlled by signals received through the B cell receptor (BCR) and follicular helper T (TFH) cell -derived signals, in particular costimulation through CD40. Here, we demon-strate that the TFH cell effector cytokine interleukin-21 (IL-21) joins BCR and CD40 in supporting BOc selection and reveal that strong IL-21 signaling prioritizes ASC differentiation in vivo. BGc cells, compared with non-BGc cells, show significantly reduced IL-21 binding and attenuated signaling, which is mediated by low cellular heparan sulfate (HS) sulfation. Mechanistically, N-deacetylase and N-sulfotransferase 1 (Ndst1)-mediated N-sul-fation of HS in B cells promotes IL-21 binding and signal strength. Ndst1 is down-regulated in BGc cells and up -regulated in ASC precursors, suggesting selective desensitization to IL-21 in BGc cells. Thus, specialized bio-chemical regulation of IL-21 bioavailability and signal strength sets a balance between the stringency and effi-ciency of GC selection.
摘要：
A unique photoelectrochemical fuel cell consisting of dual photoelectrodes is developed by utilizing light, ascorbic acid, and oxygen to produce electric power. Specifically, the integration of bifunctional single‐atom iron cocatalysts significantly facilitates anodic ascorbic acid oxidation reaction and cathodic oxygen reduction reaction, effectively improving interfacial reaction kinetics and photoelectric conversion efficiency. Abstract Semiconductor‐based photoelectrochemical (PEC) fuel cells offer a feasible solution for sustainable and environmentally friendly energy production by converting solar and chemical energy into electrical energy. However, the low PEC activities of PEC fuel cells have hindered their practical application due to rapid electron‐hole recombination and slow interfacial reaction kinetics. To address this issue, a unique PEC fuel cell composed of dual photoelectrodes utilizing low‐cost biomass, ascorbic acid, as an organic fuel is reported. Significantly, the integration of bifunctional iron single‐atom catalysts (Fe SACs) and photoactive materials has effectively constructed a bridge for charge carrier transfer, boosting interfacial reaction kinetics and photoelectric conversion efficiency. Notably, the optimal dual‐photoelectrode PEC fuel cell decorated with Fe SACs exhibits superior performance, delivering a maximum power density of 82.82 µW cm−2. Taking advantage of the peroxidase‐like activity of Fe SACs, the resultant self‐powered PEC fuel cells are explored for sensitively detecting actual uric acid samples. This study provides a promising avenue to boost the energy conversion efficiency of PEC fuel cells for sensitive self‐powered biosensing.
摘要：
LDs (Lipid droplets) are key organelles for lipid metabolism and storage, which are closely related to ferroptosis and fatty liver. Due to its small size and highly dynamic nature, developing high-fidelity fluorescent probes for imaging of LDs is crucial for observing the dynamic physiological processes of LDs and investigating LDs-associated diseases. Herein, we synthesized three dicyanoisophorone-based fluorescent probes (DCIMe, DCIJ, and DCIQ) with different electron-donating groups and studied their imaging performance for LDs. The results show that DCIQ is highly polarity sensitive and can perform high-fidelity imaging for LDs, with significantly better performance than DCIMe, DCIJ, and commercial LD probe BODIPY 493/503. Based on this, DCIQ was successfully applied to real-time observe the interplays between LDs and other organelles (mitochondria, lysosomes, and endoplasmic reticulum), and to image the dynamics of LDs with fast scanning mode (0.44s/frame) and the generation of oleic acid-induced LDs with high-fidelity. Finally, DCIQ was used to study the changes of LDs in the ferroptosis process and nonalcoholic fatty liver disease tissues. Overall, this study provided a powerful tool for high-fidelity imaging of LDs in cells and tissues.
摘要：
Inositol hexakisphosphate (IP6), a naturally occurring metabolite of inositol with specific functions in different organelles or tissues, participates in numerous physiological processes and plays a key role in mammalian metabolic regulation. However, current IP6 detection methods, i.e., high-performance liquid chromatography and gel electrophoresis, require sample destruction and lack spatiotemporal resolution. Here, we construct and characterize a genetically encoded fluorescence biosensor named HIPSer that enables ratiometric quantitative IP6 detection in HEK293T cells and subcellular compartments. We demonstrate that HIPSer has a high sensitivity and relative selectivity for IP6 in vitro. We also provide proof-of-concept evidence that HIPSer can monitor IP6 levels in real time in HEK293T cells and can be targeted for IP6 detection in the nucleus of HEK293T cells. Moreover, HIPSer could also detect changes in IP6 content induced by chemical inhibition of IP6-metabolizing enzymes in HEK293T cells. Thus, HIPSer achieves spatiotemporally precise detection of fluctuations in endogenous IP6 in live cells and provides a versatile tool for mechanistic investigations of inositol phosphate functions in metabolism and signaling.
期刊：
Journal of Controlled Release,2023年359:188-205 ISSN：0168-3659
通讯作者：
Wang, SY;Sun, Y
作者机构：
[Xiang, Chunrong; Yang, Kaiqing; Luo, Hao; Mao, Tianlong; Yu, Mengran; Cheng, Ye; Wang, Songyun; Hu, Haoyuan; Zhao, Jiahui; Wang, Jiale; Wang, Xinqi; Qin, Youran] Wuhan Univ, Renmin Hosp, Cardiac Auton Nervous Syst Res Ctr, Cardiovasc Res Inst,Dept Cardiol,Hubei Key Lab Car, Wuhan, Peoples R China.;[Ma, Kezhong] Xiangyang Cent Hosp, Dept Cardiol, Xiangyang, Peoples R China.;[Sun, Yao; Li, Qian] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensor Technol &, Natl Key Lab Green Pesticide, Wuhan, Peoples R China.;[Li, Qian] Hubei Normal Univeris, Hubei Key Lab Pollutant Anal & Reuse Technol, Huangshi, Peoples R China.;[Wang, Songyun] Wuhan Univ, Renmin Hosp, Cardiac Auton Nervous Syst Res Ctr, Cardiovasc Res Inst,Dept Cardiol,Hubei Key Lab Car, Wuhan 430061, Peoples R China.
通讯机构：
[Wang, SY ] W;[Sun, Y ] C;Wuhan Univ, Renmin Hosp, Cardiac Auton Nervous Syst Res Ctr, Cardiovasc Res Inst,Dept Cardiol,Hubei Key Lab Car, Wuhan 430061, Peoples R China.;Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensor Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.
摘要：
Phototherapy (PT), including photodynamic therapy (PDT) and photothermal therapy (PTT), has recently achieved significant advances in antitumor and antiinfection therapy. Sonodynamic therapy (SDT), as a novel noninvasive therapy with a deeper penetration depth (>8 cm), fewer side effects and non-phototoxicity than PT, has drawn much attention in recent years. However, both PT and SDT have intrinsic limitations. By combining PT with SDT, the dualmodel therapy with advanced sensitizers overcome the intrinsic limitations and show higher efficacy than traditional monotherapy. Moreover, the photo-diagnosis modality could be easily integrated into synergistic therapy so that the sensitizer acts as a tracer for fluorescence/photoacoustic imaging, and the treatment process is visualized in a way that SDT combined with other therapies cannot achieve. This review summarizes the advanced sensitizers and the application of combination therapy, and explores the improvement strategies for promoting clinical transformation.
通讯机构：
[Changlin Liu] K;Key Laboratory of Pesticide and Chemical Biology of Ministry Education, School of Chemistry, Central China Normal University, Wuhan 430079, Hubei, PR China
摘要：
Defects in mitochondrial proteostasis contribute to many disorders, including cancer, neurodegeneration, and metabolic and genetic diseases. A strategy aimed at restoring the damaged mitochondrial proteostasis is the mitochondrion-targeting and carrier-free delivery of exogenous functional proteins that can replace the endogenous dysfunctional proteins. The modification of a protein with a photolabile protecting group (PPG, i.e., photocage group) can be activated in situ by response to illumination, leading to release of the protein from its photocage. Here, the Cys and peptide photocages with coumarin were first prepared and characterized for proof of concept. Then, we designed a pair of photocage groups PPG-RhB and PPG-TPP using coumarin and mitochondrion-targeting Rhodamine B (RhB) and triphenylphosphine (TPP), and another pair of organelle-nontarget photocage groups Br-PPG and NO(2)-PPG for comparison. The proteins modified with these two pairs of photocage groups undergo photolysis in solutions, and can penetrate cell membrane toward their destinations in the carrier-free fashions. The intracellular protein photocages are in situ activated by illumination at 405nm, and the proteins are released from their photocages in mitochondria and cytoplasm, respectively. This strategy of light-responsive and carrier-free cellular delivery enables mitochondrial and cytoplasmic accumulation of exogenous proteins.
摘要：
Two-dimensional (2D) layered photocatalysts with highly ordered out-of-plane symmetry usually display robust excitonic effects, thus being ineffective in driving catalytic reactions that necessitate unchained charge carriers. Herein, taking 2D BiOBr as a prototype model, we implement a superficial asymmetric [Br-Bi-O-Bi] stacking in the out-of-plane direction by selectively stripping off the top-layer Br of BiOBr. This local asymmetry disrupts the diagnostic confinement configuration of BiOBr to urge energetic exciton dissociation into charge carriers and further contributes to the emergence of a surface dipole field that powers the subsequent separation of transient electron-hole pairs. Distinct from the symmetric BiOBr, which activates O(2) into (1)O(2) via an exciton-mediated energy transfer, surface asymmetric BiOBr favors selective O(2) activation into ·O(2)(-) for a broad range of amine-to-imine conversions. Our work here not only presents a paradigm for asymmetric photocatalyst design but also expands the toolkit available for regulating exciton behaviors in semiconductor photocatalytic systems.
摘要：
Developing a novel and potent adjuvant with great biocompatibility for immune response augmentation is of great significance to enhance vaccine efficacy. In this work, we prepared a long-term stable, pH-sensitive, and biodegradable Mn(3)(PO(4))(2)·3H(2)O nanoparticle (nano-MnP) by simply mixing MnCl(2)/NaH(2)PO(4)/Na(2)HPO(4) solution for the first time and employed it as an immune stimulant in the bivalent COVID-19 protein vaccine comprised of wild-type S1 (S1-WT) and Omicron S1 (S1-Omicron) proteins as antigens to elicit a broad-spectrum immunity. The biological experiments indicated that the nano-MnP could effectively activate antigen-presenting cells through the cGAS-STING pathway. Compared with the conventional Alum-adjuvanted group, the nano-MnP-adjuvanted bivalent vaccine elicited approximately 7- and 8-fold increases in IgG antibody titers and antigen-specific IFN-γ secreting T cells, respectively. Importantly, antisera of the nano-MnP-adjuvanted group could effectively cross-neutralize the SARS-CoV-2 and its five variants of concern (VOCs) including Alpha, Beta, Gamma, Delta, and Omicron, demonstrating that this bivalent vaccine based on S1-WT and S1-Omicron proteins is an effective vaccine design strategy to induce broad-spectrum immune responses. Collectively, this nano-MnP material may provide a novel and efficient adjuvant platform for various prophylactic and therapeutic vaccines and provide insights for the development of the next-generation manganese adjuvant.
作者机构：
[Yin, Jun; Yang, Guang-Fu; Zeng, Xiaoyan; Yang, GF; Li, Biao; Hua Liu, Sheng; Dong, Jin; Ma, Xiaoxie] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensor Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.
通讯机构：
[Yin, J; Yang, GF ] C;Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensor Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.
摘要：
4-Hydroxyphenylpyruvate dioxygenase (HPPD) plays a crucial role in the synthesis of nutrients needed to maintain optimal plant growth. Its level is closely linked to the extent of abiotic stress experienced by plants. Moreover, it is also the target of commercial herbicides. Therefore, labeling of HPPD in plants not only enables visualization of its tissue distribution and cellular uptake, it also facilitates assessment of abiotic stress of plants and provides information needed for the development of effective environmentally friendly herbicides. In this study, we created a method for fluorescence labeling of HPPD that avoids interference with the normal growth of plants. In this strategy, a perylene-linked dibenzyl-cyclooctyne undergoes strain-promoted azide-alkyne cycloaddition with an azide-containing HPPD ligand. The activation-based labeling process results in a significant emission enhancement caused by the change in the fluorescent forms from an excimer to a monomer. Notably, this activated bioorthogonal strategy is applicable to visualizing HPPD in Arabidopsis thaliana, and assessing its response to multiple abiotic stresses. Also, it can be employed to monitor in vivo levels and locations of HPPD in crops. Consequently, the labeling strategy will be a significant tool in investigations of HPPD-related abiotic stress mechanisms, discovering novel herbicides, and uncovering unknown biological functions.
作者机构：
[Zhu, Hongda; Yang, Chaobo; Yan, Aqin; Qiang, Wei; Ruan, Rui; Ma, Kai; Guan, Yeneng; Yu, Qi] Cooperative Innovation Center of Industrial Fermentation (Ministry of Education and Hubei Province), Key Laboratory of Fermentation Engineering (Ministry of Education), National '111' Center for Cellular Regulation and Molecular Pharmaceutics, School of Food and Biological Engineering, Hubei University of Technology, Wuhan, China;[Li, Jing; Zheng, Hongmei; Dai, Zhu] Hubei Cancer Hospital, Tongji Medical College, Huazhong University of Science and Technology, Wuhan, China;[Sun, Yao] Key Laboratory of Pesticide and Chemical Biology, Ministry of Education, College of Chemistry, Central China Normal University, Wuhan, China;Key Laboratory of Optic-electric Sensing and Analytical Chemistry for Life Science, Ministry of Education, Qingdao University of Science and Technology, Qingdao, China;[Liu, Shuang] School of Materials Science and Engineering, Wuhan University of Technology, Wuhan, China
摘要：
The multifunctional nano‐adjuvant Fucoidan@Al(OH)3‐Poly(I:C)/IR‐820 (FAPI) combined with photothermal and photodynamic had great application potential in the treatment of breast cancer. This therapy strategy could trigger the release of tumor antigens, enhance antitumor immunity through immunomodulation and reversal of immunosuppression, thereby achieving potent antitumor immunity, inhibiting metastasis, and enhancing antitumor effects. Abstract Photomediated immunotherapy explored to combine the anti‐cancer effect of phototherapy with the immune enhancement ability of immunotherapy, and shown great prospects for cancer treatment strategies. However, photomediated immunotherapy triggered antitumor immunity through the release of tumor antigens and damage‐associated molecular patterns from necrotic tumor cells was not enough mighty to improve the therapeutic benefits due to the immunosuppressive tumor microenvironments. Herein, a tumor‐targeted nano‐adjuvant Fucoidan@Al(OH)3‐Poly(I:C)/IR‐820 for tumor‐targeted therapy and metastasis inhibition was designed and prepared. The intrinsic immunomodulatory effects of tumor‐targeted nano‐adjuvant and their ability to simultaneously trigger tumor antigen release, thereby reversing immunosuppression and achieving potent antitumor immunity and augmented cancer therapy, were explored. The results proved that the multifunctional nano‐adjuvant combined with photothermal, photodynamic, and immunotherapy could effectively treat breast cancer and had metastasis inhibition effect by enhancing anti‐tumor immunity through immunomodulation, it should have great application potential in the treatment of breast cancer.
作者机构：
[Fu, Mingli; Li, Ying; Wang, Xinyu; Chen, Dongdong; Chen, Peirong; Xu, Xin; Ye, Daiqi] South China Univ Technol, Sch Environm & Energy, Natl Engn Lab VOCs Pollut Control Technol & Equipm, Guangdong Prov Key Lab Atmospher Environm & Pollut, Guangzhou 510006, Peoples R China.;[Li, Yongdan; Kang, Running] Aalto Univ, Sch Chem Engn, Dept Chem & Met Engn, Espoo 02150, Finland.;[Guo, Yanbing] Cent China Normal Univ, Inst Environm & Appl Chem, Coll Chem, Wuhan 430079, Peoples R China.
通讯机构：
[Peirong Chen] N;National Engineering Laboratory for VOCs Pollution Control Technology and Equipment, Guangdong Provincial Key Laboratory of Atmospheric Environment and Pollution Control, School of Environment and Energy, South China University of Technology, 510006 Guangzhou, China
作者机构：
[Pei, Qijun; Yu, Jiafeng; Qiu, Guanghao; Yu, Yang; Guo, Jianping] Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China;Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing 100049, China;[Wen, Junfeng] School of Chemistry and Chemical Engineering, Yulin University, Yulin 719000, China;[Rao, Li] Hubei International Scientific and Technological Cooperation Base of Pesticide and Green Synthesis, Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, College of Chemistry, Central China Normal University, Wuhan 430079, China;State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China
摘要：
Liquid organic hydrogen carriers (LOCHs) hold considerable potential for large-scale and long-distance energy/hydrogen storage and transportation. However, due to the lack of efficient catalysts, harsh conditions are needed for the reversible hydrogen uptake and/or release of LOHCs. Herein, a one-pot method was developed to synthesize an ultrafine metastable Ru-B alloy, where the geometrical and electronic structure of Ru is well modulated by B. To our delight, the hydrogenation of N-ethylcarbazole (NEC, one of the promising LOHC candidates) could be catalyzed by Ru-B alloy with ca. 99 % yield to 12H-NEC at room temperature. To the best of our knowledge, this is the first example of realizing the hydrogenation of NEC at room temperature. Theoretical simulations indicate that the (0001) surface of Ru7B3 crystal may be the active site for the catalytic hydrogenation. This work shows the potency of metastable nanomaterials as efficient catalysts for chemical transformations which are kinetically challenging.
