Identification of an active center of catalysts under realistic working conditions of oxygen reduction reaction (ORR) still remains a great challenge and unclear. Herein, we synthesize the Cu single atom embedded on nitrogen-doped graphene-like matrix electrocatalyst (abbreviated as SA-Cu/NG). The results show that SA-Cu/NG possesses a higher ORR capability than 20% Pt/C at alkaline solution while the inferior activity to 20% Pt/C at acidic medium. Based on the experiment and simulation calculation, we identify the atomic structure of Cu-N₂C₂ in SA-Cu/NG and for the first time unravels that the oxygen-reconstituted Cu-N₂C₂-O structure is really the active species of alkaline ORR, while the oxygen reconstitution does not happen at acidic medium. The finding of oxygen-reconstituted active species of SA-Cu/NG at alkaline media successfully unveils the bottleneck puzzle of why the performance of ORR catalysts at alkaline solution is better than that at acidic media, which provides new physical insight into the development of new ORR catalysts.

Early cancer diagnosis and treatment are crucial research fields of human health. One method that has proven efficient is biomarker detection which can provide real-time and accurate biological information for early diagnosis. This review presents several biomarker sensors based on electrochemistry, surface plasmon resonance (SPR), nanowires, other nanostructures, and, most recently, metamaterials which have also shown their mechanisms and prospects in application in recent years. Compared with previous reviews, electrochemistry-based biomarker sensors have been classified into three strategies according to their optimizing methods in this review. This makes it more convenient for researchers to find a specific fabrication method to improve the performance of their sensors. Besides that, as microfabrication technologies have improved and novel materials are explored, some novel biomarker sensors—such as nanowire-based and metamaterial-based biomarker sensors—have also been investigated and summarized in this review, which can exhibit ultrahigh resolution, sensitivity, and limit of detection (LoD) in a more complex detection environment. The purpose of this review is to understand the present by reviewing the past. Researchers can break through bottlenecks of existing biomarker sensors by reviewing previous works and finally meet the various complex detection needs for the early diagnosis of human cancer.

The emerging antimicrobial resistance (AMR) poses serious threats to the global public health. Conventional antibiotics have been eclipsed in combating with drug-resistant bacteria. Moreover, the developing and deploying of novel antimicrobial drugs have trudged, as few new antibiotics are being developed over time and even fewer of them can hit the market. Alternative therapeutic strategies to resolve the AMR crisis are urgently required. Pathogen-oriented therapy (POT) springs up as a promising approach in circumventing antibiotic resistance. The tactic underling POT is applying antibacterial compounds or materials directly to infected regions to treat specific bacteria species or strains with goals of improving the drug efficacy and reducing nontargeting and the development of drug resistance. This review exemplifies recent trends in the development of POTs for circumventing AMR, including the adoption of antibiotic-antibiotic conjugates, antimicrobial peptides, therapeutic monoclonal antibodies, nanotechnologies, CRISPR-Cas systems, and microbiota modulations. Employing these alternative approaches alone or in combination shows promising advantages for addressing the growing clinical embarrassment of antibiotics in fighting drug-resistant bacteria.

Environment-friendly protic amine carboxylic acid ionic liquids (ILs) as solvents is a significant breakthrough with respect to traditional highly coordinating and toxic solvents in achieving efficient and stable perovskite solar cells (PSCs) with a simple one-step air processing and without an antisolvent treatment approach. However, it remains mysterious for the improved efficiency and stability of PSCs without any passivation strategy. Here, we unambiguously demonstrate that the three functions of solvents, additive, and passivation are present for protic amine carboxylic acid ILs. We found that the ILs have the capability to dissolve a series of perovskite precursors, induce oriented crystallization, and chemically passivate the grain boundaries. This is attributed to the unique molecular structure of ILs with carbonyl and amine groups, allowing for strong interaction with perovskite precursors by forming C=O…Pb chelate bonds and N-H…I hydrogen bonds in both solution and film. This finding is generic in nature with extension to a wide range of IL-based perovskite optoelectronics.

The dialogue system has always been one of the important topics in the domain of artificial intelligence. So far, most of the mature dialogue systems are task-oriented based, while non-task-oriented dialogue systems still have a lot of room for improvement. We propose a data-driven non-task-oriented dialogue generator “CERG” based on neural networks. This model has the emotion recognition capability and can generate corresponding responses. The data set we adopt comes from the NTCIR-14 STC-3 CECG subtask, which contains more than 1.7 million Chinese Weibo post-response pairs and 6 emotion categories. We try to concatenate the post and the response with the emotion, then mask the response part of the input text character by character to emulate the encoder-decoder framework. We use the improved transformer blocks as the core to build the model and add regularization methods to alleviate the problems of overcorrection and exposure bias. We introduce the retrieval method to the inference process to improve the semantic relevance of generated responses. The results of the manual evaluation show that our proposed model can make different responses to different emotions to improve the human-computer interaction experience. This model can be applied to lots of domains, such as automatic reply robots of social application.

Developing efficient seawater-electrolysis system for mass production of hydrogen is highly desirable due to the abundance of seawater. However, continuous electrolysis with seawater feeding boosts the concentration of sodium chloride in the electrolyzer, leading to severe electrode corrosion and chlorine evolution. Herein, the common-ion effect was utilized into the electrolyzer to depress the solubility of NaCl. Specifically, utilization of 6 M NaOH halved the solubility of NaCl in the electrolyte, affording efficient, durable, and sustained seawater electrolysis in NaCl-saturated electrolytes with triple production of H₂, O₂, and crystalline NaCl. Ternary NiCoFe phosphide was employed as a bifunctional anode and cathode in simulative and Ca/Mg-free seawater-electrolysis systems, which could stably work under 500 mA/cm² for over 100 h. We attribute the high stability to the increased Na⁺ concentration, which reduces the concentration of dissolved Cl^- in the electrolyte according to the common-ion effect, resulting in crystallization of NaCl, eliminated anode corrosion, and chlorine oxidation during continuous supplementation of Ca/Mg-free seawater to the electrolysis system.

The intrinsically rigid and limited strain of most conjugated polymers has encouraged us to optimize the extensible properties of conjugated polymers. Herein, learning from the hydrogen bonds in glucose, which were facilitated to the toughness enhancement of cellulose, we introduced interchain hydrogen bonds to polydiarylfluorene by amide-containing side chains. Through tuning the copolymerization ratio, we systematically investigated their influence on the hierarchical condensed structures, rheology behavior, tensile performances, and optoelectronic properties of conjugated polymers. Compared to the reference copolymers with a low ratio of amide units, copolymers with 30% and 40% amide units present a feature of the shear-thinning process that resembled the non-Newtonian fluid, which was enabled by the interchain dynamic hydrogen bonds. Besides, we developed a practical and universal method for measuring the intrinsic mechanical properties of conjugated polymers. We demonstrated the significant impact of hydrogen bonds in solution gelation, material crystallization, and thin film stretchability. Impressively, the breaking elongation for P4 was even up to ~30%, which confirmed the partially enhanced film ductility and toughness due to the increased amide groups. Furthermore, polymer light-emitting devices (PLEDs) based on these copolymers presented comparable performances and stable electroluminescence (EL). Thin films of these copolymers also exhibited random laser emission with the threshold as low as 0.52  μJ/cm², suggesting the wide prospective application in the field of flexible optoelectronic devices.

Fluorescence probes with aggregation-induced emission (AIE) characteristics are of great importance in biomedical imaging with superior spatial and temporal resolution. However, the lack of toxicity studies and deep tissue imaging in nonhuman primates hinders their clinical translation. Here, we report the blood chemistry and histological analysis in nonhuman primates treated with AIE probes over tenfold of an intravenous dose of clinically used indocyanine green (ICG) during a study period of 36 days to demonstrate AIE probes are nontoxic. Furthermore, through bright and nontoxic AIE probes and fluorescence imaging in the second window (NIR-II, 1,000–1,700 nm), we achieve an unprecedented 1.5-centimeter-deep vascular imaging in nonhuman primates, breaking the current limitation of millimeter-deep NIR-II fluorescence imaging. Our important findings, i.e., nontoxic features of AIE probes and centimeter-deep NIR-II vascular imaging in nonhuman primates, may facilitate successful translation of AIE probes in clinical trials.

Organic-inorganic halide perovskites (OIHPs) are recognized as the promising next-generation X-ray detection materials. However, the device performance is largely limited by the ion migration issue of OIHPs. Here, we reported a simple atomistic surface passivation strategy with methylammonium iodide (MAI) to remarkably increase the ion migration activation energy of CH₃NH₃PbI₃ single crystals. The amount of MAI deposited on the crystal surface is finely regulated by a self-assemble process to effectively suppress the metallic lead defects, while not introducing extra mobile ions, which results in significantly improved dark current stability of the coplanar-structure devices under a large electric field of 100 V mm^-1. The X-ray detectors hence exhibit a record-high sensitivity above 700,000  μC  {\text{Gy}}_{\text{air}}^{‐1} cm^‐2 under continuum X-ray irradiation with energy up to 50 keV, which enables an ultralow X-ray detection limit down to 1.5 nGy_air s^-1. Our findings will allow for the dramatically reduced X-ray exposure of human bodies in medical imaging applications.

Photocleavable hydrogels are of great importance in the field of controlled drug delivery, stem cell fate regulation, surface patterning, and intelligent devices. However, the development of novel photocleavable gel systems by visible light is usually met with challenges such as the lack of efficient and tunable photocleavable groups and reactions. Herein, we reported the facile fabrication of a new type of photocleavable hydrogels by the direct gelation of 4-arm thiol-terminated polyethylene glycol with 3,6-dichloro-1,2,4,5-tetrazine via the formation of S,S-tetrazine linkages. The prepared hydrogels underwent efficient degradation upon irradiation by ultraviolet or green light, and the degradation kinetics could be significantly promoted by hydrogen peroxide. Correspondingly, the hydrogels loaded with calcium peroxide microparticles or glucose oxidase/catalase enzymes enabled the precise and efficient in vivo photocontrol of gel degradation and drug release for cancer treatment. This work offers a promising and facile strategy towards the fabrication of visible light cleavable hydrogels with tunable and on-demand drug release properties.