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Electrochemical reduction of CO2 is an important way to achieve carbon neutrality, and much effort has been devoted to the design of active sites. Apart from elevating the intrinsic activity, expanding the functionality of active sites may also boost catalytic performance. Here we designed "negatively charged Ag (nc‐Ag)" active sites featuring both the intrinsic activity and the capability of regulating microenvironment, through modifying Ag nanoparticles with atomically dispersed Sn species. Different from conventional active sites (which only mediate the surface processes by bonding with the intermediates), the nc‐Ag sites could also manipulate environmental species. Therefore, the sites could not only activate CO2, but also regulate interfacial H2O and CO2, as confirmed by operando spectroscopies. The catalyst delivers a high current density with a CO faradaic efficiency of 97 %. Our work here opens up new opportunities for the design of multifunctional electrocatalytic active sites. [ABSTRACT FROM AUTHOR]

Comprehensive Summary: Nano‐catalysis plays a vital role in the industrially chemical transformations. The increasingly severe energy crisis and environmental issues spur scientists to exploit novel nano‐catalysts in diverse fields. It is essential to understand the fundamental physicochemical properties of nano‐catalysts to develop efficient systems, whose design can be subsequently precisely tuned at the atomic level. In this review, we summarize several key factors affecting the catalytic activity of nano‐catalysts, including structure, composition, size, and interface, providing guidance for the atomic level control of high‐efficient nano‐catalysts. Finally, we present a brief conclusion and some thoughts on nano‐catalysis. What is the most favorite and original chemistry developed in your research group? Nanomaterials for catalysis and renewable energy. How do you supervise your students? I always encourage my students to innovate, persist and enjoy their researches. What is the most important personality for scientific research? Strong interest. What are your hobbies? What's your favorite book(s)? Reading, travelling and gaming. My favorite books are novels that give me a variety of different experiences. How do you keep balance between research and family? I always try to make time to be with my family, however busy I am. [ABSTRACT FROM AUTHOR]

The development of highly active and stable bifunctional noble‐metal‐based electrocatalysts for the hydrogen evolution reaction (HER) and the oxygen evolution reaction (OER) is a crucial goal for clean and renewable energy, which still remains challenging. Herein, we report an efficient and stable catalyst comprising a Co single atom incorporated in an RuO2 sphere for HER and OER, in which the Co single atom in the RuO2 sphere was confirmed by XAS, AC‐STEM, and DFT. This tailoring strategy uses a Co single atom to modify the electronic structures of the surrounding Ru atoms and thereby remarkably elevates the electrocatalytic activities. The catalyst requires ultralow overpotentials, 45 mV for HER and 200 mV for OER, to deliver a current density of 10 mA cm−2. The theoretical calculations reveal that the energy barriers for HER and OER are lowered after incorporation of a cobalt single atom. [ABSTRACT FROM AUTHOR]

For electrocatalysts for the hydrogen evolution reaction (HER), encapsulating transition metal phosphides (TMPs) into nitrogen‐doped carbon materials has been known as an effective strategy to elevate the activity and stability. Yet still, it remains unclear how the TMPs work synergistically with the N‐doped support, and which N configuration (pyridinic N, pyrrolic N, or graphitic N) contributes predominantly to the synergy. Here we present a HER electrocatalyst (denoted as MoP@NCHSs) comprising MoP nanoparticles encapsulated in N‐doped carbon hollow spheres, which displays excellent activity and stability for HER in alkaline media. Results of experimental investigations and theoretical calculations indicate that the synergy between MoP and the pyridinic N can most effectively promote the HER in alkaline media. [ABSTRACT FROM AUTHOR]

We report a family of cationic lead halide layered materials, formulated as [Pb2X2]2+[−O2C(CH)2CO2−] (X=F, Cl, Br), exhibiting pronounced broadband white-light emission in bulk form. These well-defined PbX-based structures achieve an external quantum efficiency as high as 11.8 %, which is comparable to the highest reported value (ca.9 %) for broadband phosphors based on layered organolead halide perovskites. More importantly, our cationic materials are ultrastable lead halide materials, which overcome the air/moisture-sensitivity problems of lead perovskites. In contrast to the perovskites and other bulk emitters, the white-light emission intensity of our materials remains undiminished after continuous UV irradiation for 30 days under atmospheric conditions (ca.60 % relative humidity). Our mechanistic studies confirm that the broadband emission is ascribed to short-range electron-phonon coupling in the strongly deformable lattice and generated self-trapped carriers. [ABSTRACT FROM AUTHOR]