• Energy Research

Ammonia (NH3) is a vital chemical for modern human society. It is conventionally produced by the energy‐ and emission‐intensive Haber–Bosch process. Alternatively, sustainable NH3 production from renewable electricity‐driven electrolyzers has emerged as a promising route. Particularly, NH3 synthesis from nitrate (NO3−), a common pollutant in water and soil, by the nitrate reduction reaction (NO3RR) has drawn wide attention. Among various catalysts demonstrated recently, copper (Cu)‐based catalysts have been recognized as attractive candidates due to their availability, good activity, high NH3 selectivity, and facile reaction kinetics. In this review, the recent progress of Cu‐based NO3RR catalysts from the reaction mechanistic fundamentals to various catalyst design strategies, aiming at providing an on‐time summary, is summarized, and perspectives that can guide the rational and on‐demand design of Cu‐ and other earth‐abundant metal‐based catalysts for selective NO3RR toward sustainable NH3 production are elucidated.

This review summarizes the latest advances in hydrogen evolution reaction under neutral conditions to enlighten future researches.

Rechargeable aqueous zinc-ion batteries (AZIBs) have attracted interest in serving as large-scale electrochemical energy storage devices because of their high energy storage capacity, low cost, outstanding operational safety, and superior environmental friendliness. In the past two decades, enormous efforts have been devoted to all components of AZIBs, including cathode materials, Zn anodes, and electrolytes. This brief review first outlines the challenges of realizing practical ZIBs for cathodes, anodes, and electrolytes. Then, we focus on recent representative and promising electrolyte addictive studies. We further present our perspectives on critical issues to be addressed to enable practical AZIBs.

Heterogeneous molecular catalysts built from β-substituted cobalt porphyrins and carbon nanotubes afford tunable activity for H2O2 synthesis via the two-electron transfer oxygen reduction reaction.

Abstract Translating the advantages of carbon nanomaterials into macroscopic energy storage devices is challenging because the desirable nanoscale properties often disappear during assembly processes. Here we describe a new nonequilibrium subcritical hydrothermal method capable of independently manipulating the temperature and pressure to create unique assembly conditions crossing the commonly used liquid-vapor boundary. Highly conductive and dense-packed yet ion-accessible nanocarbon microfibers can be obtained from graphene oxide sheets, single-walled carbon nanotubes, and a nitrogen-doping crosslinker under 20 min of hydrothermal assembly, 80% energy saving compared to standard hydrothermal methods, and one of the shortest time in the field of hydrothermal processing of carbon nanomaterials. Using those microfibers, we built microsupercapacitors that reach a high volumetric capacitance of 52 F cm−3, energy density of 7.1 mWh cm−3, and power density of 1645.7 mW cm−3, respectively. We further demonstrate the 3D integration of multiple fiber microsupercapacitors that reduces the device footprint by 75% while expanding the operational voltage and current window. This strategy is a promising tool for harmoniously assembling carbon nanostructures as energy storage components for various energy applications.

Customized hybrid carbon fiber supercapacitors with energy across two orders and power across four orders of magnitude.

Lithium (Li) production based on the soda evaporation process is time-consuming and unsustainable. The emerging electrochemical Li extraction is time-efficient but requires high-concentration Li sources and significant electrical energy input. Here, we demonstrate a fast, energy-saving, and environment-friendly Li production process by coupling a thermally regenerative electrochemical cycle (TREC) using lithium manganese oxide (LMO) and nickel hexacyanoferrate (NiHCF) electrodes with poly(vinylidene fluoride) membrane-based thermo-osmosis (denoted as TO-TREC). The characterization of LMO and NiHCF electrodes confirmed that the relatively high temperature of TO-TREC has negligible adverse effects on the ion intercalation in LMO and NiHCF electrodes. The LMO/NiHCF pair has a positive temperature coefficient of 0.843 mV K-1. In the TO-TREC process, Li ions are selectively extracted from a Li-containing brine warmed by low-grade heat and then released into a room-temperature recovery solution such as LiCl with a production rate of 50-60 mmol Li+ m-2 h-1. Li source solutions are concentrated by thermo-osmosis simultaneously, making it possible to utilize previously unusable Li-containing sources, such as concentrated brines from desalination plants and industrial effluents. Besides, the TREC harvests thermal energy from the heated brine, saving >20% of electrical energy compared to conventional electrochemical methods. The new process shows the potential to meet the growing global Li demands for many applications.

AbstractSynthesis of structurally controlled graphene materials is critical for realizing their practical applications. The electrochemical exfoliation of graphite has emerged as a simple method to produce graphene materials. This review examines research progress in the last 5 years, from 2015 to 2019. Graphene material synthesis methods generally have a trade‐off between increasing production yield and achieving better material property control. The synthesis conditions for synthesizing pristine graphene, graphene oxide (GO), and graphene composites are significantly different. Thus, in this review, we first discuss synthesis methods for graphene materials with high C/O ratios from four aspects: graphite electrodes, equipment engineering, electrolytes, and additional reduction methods. Next, we survey synthesis methods for GO and examine how the pretreatment of the graphite electrodes, electrolytes, and operation parameters, such as applied voltages, electrolyte temperatures, and mechanical forces, affect the quality of GO. Further, we summarize electrochemical exfoliation methods used to dope graphene materials, introduce covalent functional groups, incorporate various nanoparticles, and assembly of graphene architectures. For all synthesis methods, we compare the properties of resulting graphene materials such as C/O ratios, lateral size, layer numbers, and quality characterized by Raman spectroscopy. Lastly, we propose our perspectives on further research. We hope this review stimulates more studies to realize the on‐demand production of graphene materials with desired properties using electrochemical exfoliation methods.